DEVELOPMENT DOCUMENT

                     for

EFFLUENT LIMITATIONS GUIDELINES AND STANDARDS

                   for the

     COPPER FORMING POINT SOURCE CATEGORY
               Anne M. Gorsuch
                Administrator
            Frederick A. Eidsness
      Assistant Administrator for Water
               Steven Schatzow
                   Director
  Office of Water Regulations and Standards
          Jeffery D.  Denit,  Director
         Effluent Guidelines Division
          Ernst P.  Hall,  P.E.,  Chief
         Metals and Machinery Branch
                 David Pepson
          Technical Project Officer
                 October 1982
     U.S.  Environmental Protection Agency
               Office  of Water
  Office  of Water  Regulations  and Standards
         Effluent  Guidelines  Division
           Washington,  D.C.   20460

-------
11 !.''(y  1	t  •	I'll

-------
                        TABLE OF CONTENTS
Section



I



II
III
          Title                                   Page



SUMMARY AND CONCLUSIONS	      1



RECOMMENDATIONS	      3



BPT	      3



BAT	      9



NSPS	    13



PSES	    20



PSNS  . . . .	    26



ALTERNATIVE BAT AND PSES  .	    31





INTRODUCTION	    41



LEGAL BACKGROUND	    41



BPT Effluent Limitations	    43



BAT Effluent Limitations  .	  .    44



BCT Effluent Limitations  	  ......    45



New Source Performance Standards	    45



Pretreatment Standards for Existing Sources...    46



Pretreatment Standards for New Sources  	    46



DATA GATHERING	    47



OVERVIEW OF THE INDUSTRY  ............    48



Products and Product Uses	    48



Raw Materials	    49



MANUFACTURING PROCESSES	    50



Hot Rolling	    51



Cold Rolling	    52

-------
Section
IV
V
        TABLE OF CONTENTS (Continued)



          Title                  !                 Page

Extrusion	?	    52

Drawing	•	    52

Forging	»	    53

Annealing	>	    53

Pickling	 . . .  . j,	    54
                                 i
Alkaline Cleaning	    55

Solution Heat Treatment	;.	    56

INDUSTRY SUBCATEGORIZATION ....  	    63

Raw Materials	'•	    63

Final Products	    63

Plant Size	    64

Plant Age. .	j	    64

Geographical Location	    65

Manufacturing Processes	    65

Non-Water Quality Factors. .  .	    65

Production Normalizing  Parameter 	    66

Selection of the Production Normalizing
Parameter	    67

WATER USE AND WASTEWATER CHARACTERISTICS  ....    69

SAMPLING AND ANALYTICAL PROGRAM. 	    69

Site Selection	    70
                                 I
Pollutants Analyzed	:	«  •    70
                                 ]
Sampling Methodology	'	•  •    71

Analytical Methods	;	«  •    71
                                ii

-------
 Section
VI
         TABLE OF CONTENTS  (Continued)


           Title                                   Page

 WASTEWATER SOURCES	    72

 Hot Rolling Spent Lubricant	    74

 Cold Rolling Spent Lubricant 	    74

 Drawing Spent Lubricants ..... 	    74

 Solution Heat Treatment	    74

 Extrusion Press  Solution Heat Treatment	    75

 Alkaline Cleaning Bath 	    75

 Alklaine Cleaning Rinse.  .  .,	    75

 Annealing Water	    75

 Annealing Oil	„	    75

 Pickling Baths  	    75

 Pickling Rinse  	    75

 Pickling Fume Scrubber  	    75

 PRODUCTION NORMALIZED FLOWS.  .	       75

 POLLUTANTS FOUND AND SOURCES  OF  THESE
 POLLUTANTS	    77

 Toxic Metals	       77

 Toxic Organics	     77

 Conventional Pollutants.  .	     78

 SELECTION  OF POLLUTANT PARAMETERS	   177

RATIONALE  FOR SELECTION OF POLLUTANT PARAMETERS.   178

DESCRIPTION OF POLLUTANT PARAMETERS	   179

POLLUTANT  SELECTION FOR COPPER FORMING WASTE
STREAMS	   219
                               iii

-------
Section
VII
        TABLE OF CONTENTS (Continued)




          Title                 I                  Pa§e


CONTROL AND TREATMENT TECHNOLOGY	 .  •   227


END-OF-PIPE TREATMENT TECHNOLOGIES 	   227

                                i	    	 OO Q
MAJOR TECHNOLOGIES	........   ^s


Chemical Reduction of Chromium	   228


Chemical Precipitation 	 	   230


Cyanide Precipitation	   236


Granular Bed Filtration.	   237


Pressure Filtration.	   241



Settling .	:	   243


Skimming	;	   245


Chemical Emulsion Breaking  .  .	   249
                          «      j

Thermal Emulsion Breaking.  ... 	   251


MAJOR  TECHNOLOGY EFFECTIVENESS  . 	   253


L&S  Performance - Combined  Metals  Data Base.  .  .   253



One-Day Effluent Values.	   254


Average Effluent Values	;	   257


Application	J  . .	   259


Additional Pollutants	•	   260


LS&F Performance	•  •'	    2^2


Analysis  of Treatment  System Effectiveness .  .  .    263
                                iv

-------
                  TABLE OF CONTENTS (Continued)

Section             Title                                   page
          MINOR TECHNOLOGIES 	 ......   266
          Carbon Adsorption. .  .  .	   266
          Flotation	   268
          Centrifugation ....  	  .....   270
          Coalescing	   272
          Cyanide Oxidation by  Chlorine	   274
          Cyanide Oxidation by  Ozone 	 275
          Cyanide Oxidation by  Ozone with UV Radiation .  .   276
          Cyanide Oxidation by  Hydrogen Peroxide  	   277
          Evaporation		   278
          Gravity Sludge Thickening	   281
          Ion Exchange  .............  	   282
          Insoluble  Starch Xanthate	   285
          Peat Adsorption	   285
          Membrane Filtration	   287
          Reverse Osmosis	   289
          Sludge  Bed  Drying	   292
          Ultrafiltration	    294
          Vacuum  Filtration	    296
          IN-PLANT CONTROL  TECHNIQUES  (FLOW REDUCTION)  .  .    297
          Recycle.	    298
          Alternative Rinsing Techniques  	    300
          Countercurrent Cascade Rinsing  	    301

-------
                  TABLE OF CONTENTS (Continued)
Section
VIII
          Title                                   Page

Spray Rinsing	*	   304

Contract Hauling 	

Reduction of Water Use 	

Current Industry Practice. .  .	   306

COST OF WASTEWATER TREATMENT AND CONTROL ....   375

COST ESTIMATES FOR INDIVIDUAL TREATMENT
TECHNOLOGIES	[	   375

Introduction	   375

Cost Factors and Adjustments  . ;	   377

Items Not Included in Cost Estimates	   378

System Cost Assumptions.	   378

Lime Precipitation and Clarification  	   379

Vacuum Filtration	   38°

Oil Skimming	   381

Chemical Emulsion Breaking  .	   382

Chromium Reduction	   383

Contract Hauling 	   38^

Spray Rinsing	   384

Recycle-Cooling	   38^

Multimedia  Filtration	   385

COST ESTIMATING METHODOLOGY.  . •	   385

COSTS FOR TREATMENT  AND  CONTROL OPTIONS.  ....   387

Option  1  	  .........   387

Option  2	'	   388
                                vi

-------
Section
IX
X
        TABLE OF CONTENTS (Continued)


          Title                           _        Page

Option 3	   388

Option 4	   388

Option 5	   388

NORMAL PLANT COSTS 	   388

ENERGY AND NON-WATER QUALITY ASPECTS ......   389

BEST PRACTICABLE CONTROL TECHNOLOGY CURRENTLY
AVAILABLE	. . . .	   415

TECHNICAL APPROACH TO BPT	   415

REGULATED POLLUTANT PARAMETERS 	   417

DISCHARGE FLOWS.	   418

Treatment Train	   421

Effluent Limitations 	 	   421

Compliance Costs and Environmental Benefits. .  .   422

BEST AVAILABLE  TECHNOLOGY ECONOMICALLY
ACHIEVABLE	   431

TECHNICAL APPROACH TO BAT	   431

OPTION 1 ....... 	   433

OPTION 2	   433

OPTION 3		   434

OPTION 4	   434

OPTION 5	   434

BAT OPTION SELECTION 	   434

REGULATED POLLUTANT PARAMETERS 	   435

DISCHARGE FLOWS.	   435
                              vii

-------
                  TABLE OF CONTENTS  (Continued)


Section             Title                                   Page

          Treatment Train. .  .  .	   436

          Effluent Limitations	  .   437

          Benefits	   437

XI        NEW SOURCE PERFORMANCE  STANDARDS ,	   451

          TECHNICAL APPROACH  TO NSPS	   451

          NSPS OPTION SELECTION	;.	   452

          REGULATED POLLUTANT PARAMETERS  . i.	   452

          DISCHARGE FLOWS	   453

          COSTS AND ENVIRONMENTAL BENEFITS ........   453

          EFFLUENT STANDARDS	   454

XII       PRETREATMENT STANDARDS	   461

          DISCHARGE OF COPPER FORMING WASTEWATERS TO
          A POTW	   461

          TECHNICAL APPROACH  TO PRETREATMENT  	   463

          PSES OPTION SELECTION	   464

          PSNS OPTION SELECTION	   465

          COSTS AND ENVIRONMENTAL BENEFITS OF PSES
          AND PSNS	,	   466

          REGULATED POLLUTANT PARAMETERS  	   466

          EFFLUENT STANDARDS  	 ........   466

XIII      BEST CONVENTIONAL POLLUTANT CONTROL TECHNOLOGY  .   481

XIV       ACKNOWLEDGEMENTS	,	   483

XV        GLOSSARY	,	   485

XVI       REFERENCES	,	   497
                              viii

-------
                          LIST OF FIGURES


 Number         Title                                        page

 III-l      DISTRIBUTION OF THE COPPER FORMING INDUSTRY
           BY EPA REGION	    58

 VII-1      HEXAVALENT CHROMIUM REDUCTION WITH SULFUR
           DIOXIDE.	   308

 VII-2      COMPARATIVE SOLUBILITIES  OF METAL HYDROXIDES
           AND SULFIDE AS  A FUNCTION OF pH.  .	   309

 VII-3      EFFLUENT  ZINC CONCENTRATION VS. MINIMUM
           EFFLUENT  pH	   310

 VII-4      LEAD SOLUBILITY IN THREE  ALKALIES	   311

 VII-5      FILTER CONFIGURATIONS	   312

 VII-6      GRANULAR  BED FILTRATION	   313

 VII-7      REPRESENTATIVE  TYPES OF SEDIMENTATION.  .  .  .  .  .   314

 VII-8      GRAVITY OIL-WATER SEPARATOR.  ...  	   315
                  *        .            .':       ;       - -  >
 VII-9      RELATIONSHIP BETWEEN TOTAL  TOTAL  ORGANICS  (TTS)
           AND OIL AND GREASE CONCENTRATIONS.	   316

 VII-10     FLOW DIAGRAM FOR  EMULSION BREAKING WITH
           CHEMICALS	  .  . '.  .  ...  .    317

 VII-11     HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - CADMIUM.	    318

 VII-12     HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - CHROMIUM  	    319

 VII-13     HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - COPPER  	  .....    320

VII-14     HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - LEAD	    321

VII-15    HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - NICKEL  AND ALUMINUM. ......    322

VII-16    HYDROXIDE  PRECIPITATION SEDIMENTATION
           EFFECTIVENESS - ZINC	    323
                               3.X

-------
LIST OF FIGURES  (Continued)
Number
VII-17

VII-18

VII-19

VII-20

VII-21
VII-22
VII-23
VII-24

VII-25
VII-26
VII-27
VII-28
VII-29
VII-30
VII-31
VII-32
VII-33
VII-34

VII-35
VII-36

Title
HYDROXIDE PRECIPITATION SEDIMENTATION
EFFECTIVENESS - IRON 	 	 	
HYDROXIDE PRECIPITATION SEDIMENTATION
EFFECTIVENESS - MANGANESE. ... 	
HYDROXIDE PRECIPITATION SEDIMENTATION
EFFECTIVENESS - TSS 	 	
FLOW DIAGRAM OF ACTIVATED CARBON ADSORPTION
WITH REGENERATION. . 	 	 	
ACTIVATED CARBON ADSORPTION COLUMN 	
DISSOLVED AIR FLOATION 	 1 	
CENTRIFUGATION 	 	
TREATMENT OF CYANIDE WASTE BY ALKALINE
CHLORINATION 	
TYPICAL OZONE PLANT FOR WASTE TREATMENT 	
UV/OZONATION 	
TYPES OF EVAPORATION EQUIPMENT . 	
GRAVITY THICKENING 	 	
ION EXCHANGE WITH REGENERATION . 	
SIMPLIFIED REVERSE OSMOSIS SCHEMATIC 	
REVERSE OSMOSIS MEMBRANE CONFIGURATIONS 	
SLUDGE DRYING BED. 	 	 	
SIMPLIFIED ULTRAFILTRATION FLOW SCHEMATIC. . . .
FLOW DIAGRAM FOR A BATCH TREATMENT ULTRA-
FILTRATION SYSTEM. 	 	
VACUUM FILTRATION 	 1 	
FLOW DIAGRAM FOR RECYCLING WITH A COOLING
TOWER 	 	
Page

324

325

326

327
328
329
330

331
332
333
334
335
336
337
338
339
340

341
342

343
            X

-------
LIST OF FIGURES (Continued)
Number
VII -37
VII-38
VIII-1

VIII-2
VIII-3
VIII-4

VIII-5
VIII-6
VIII-7
VIII-8
VIII-9
VIII-10
VIII-11
VIII-12

VIII-13

VIII-14
VIII-15

VIII-16
VIII-17
VIII-18
VIII-19
Title
COUNTER CURRENT RINSING (TANKS). . . 	
EFFECT OF, ADDED RINSE STAGE ON WATER USE ....
CLARIFICATION CAPTIAL COST FOR CONTINUOUS
OPERATION 	 	
CLARIFICATION CAPITAL COST FOR BATCH OPERATION .
CLARIFICATION COST SUMMARY 	
CLARIFICATION MAN HOUR REQUIREMENTS FOR
CONTINUOUS OPERATION 	 . 	
VACUUM FILTRATION CAPITAL COST 	 	
VACUUM FILTRATION LABOR REQUIREMENTS 	
VACUUM FILTRATION MATERIAL AND SUPPLY COST . . .
VACUUM FILTRATION ELECTRICAL COST. 	
OIL SKIMMER CAPITAL COST 	
OIL SKIMMER ANNUAL LABOR REQUIREMENTS 	
CHEMICAL EMULSION BREAKING INVESTMENT COSTS. . .
CHEMICAL EMULSION BREAKING OPERATION AND
MAINTENANCE COSTS. 	 . 	
ANNUAL ENERGY COSTS VS. FLOW RATE FOR
CHEMICAL EMULSION BREAKING 	
CHEMICAL REDUCTION OF CHROMIUM CAPITAL COST. . .
CHEMICAL REDUCTION OF CHROMIUM ANNUAL LABOR
REQUIREMENTS 	
HOLDING TANK INVESTMENT COSTS 	 	
COOLING TOWER CAPITAL COST 	
COOLING TOWER ANNUAL ELECTRICAL COST 	
MULTIMEDIA FILTER COSTS 	
Page
344
345

393
394
395

396
397
398
399
400
401
402
403

404

405
406

407
408
409
410
411

-------
                   LIST OF FIGURES  (Continued)
Number         Title
IX-1      BPT TREATMENT TRAIN.  .  .
X-l       OPTION 1 TREATMENT TRAIN
X-2       OPTION 2 TREATMENT TRAIN
X-3       OPTION 3 TREATMENT TRAIN
X-4       OPTION 4 TREATMENT TRAIN
X-5       OPTION 5 TREATMENT TRAIN
Page
 423
 438
 439
 440
 441
 442
                              xii

-------
                           LIST OF TABLES
 Number
 III-l

 III-2

 III-3
 III-4

 V-l
 V-2
 V-3
 V-4
 V-5
 V-6
 V-7
 V-8
 V-9
 V-10
 V-ll
 V-12
 V-13
V-14
V-15
V-16
V-17
      Title
 GEOGRAPHIC DISTRIBUTION OF COPPER FORMING
 INDUSTRY IN THE UNITED STATES BY EPA REGIONS .  .
Page

  59
 DISTRIBUTION OF  COPPER FORMING INDUSTRY
 PRODUCTS	     60
 FORMED  COPPER PRODUCT  USAGE  DISTRIBUTION ....     61
 NUMBER  OF  PLANTS  PRACTICING  VARIOUS
 MANUFACTURING OPERATIONS  IN  THE COPPER
 FORMING INDUSTRY  .........  	     62
 LIST OF 129  TOXIC POLLUTANTS	     79
 HOT ROLLING  LUBRICANT.  .	     84
 COLD ROLLING LUBRICANT  	     85
 DRAWING LUBRICANT	     86
 SOLUTION HEAT TREATMENT.	     89
 EXTRUSION  PRESS SOLUTION  HEAT  TREATMENT	     90
 ALKALINE CLEANING BATH  	     91
 ALKALINE CLEANING RINSE	     92
ANNEALING WATER	     93
ANNEALING OIL	     95
 PICKLING BATH	     96
 PICKLING RINSE 	     97
 PICKLING FUME SCRUBBER  	     99
SUMMARY OF SAMPLING DATA FROM PLANT 47432. . .  .   100
SUMMARY OF SAMPLING DATA FROM PLANT 28044. . .  .   109
SUMMARY OF SAMPLING DATA FROM PLANT 37032. ...   112
SUMMARY OF SAMPLING DATA FROM PLANT 36096. ...   121
                              xiii

-------
                    LIST OF TABLES  (Continued)
Number         Title

V-18      SUMMARY OF SAMPLING DATA FROM PLANT 1053  .  .

V-19      SUMMARY OF SAMPLING DATA FROM PLANT 19019.  .

V-20      SUMMARY OF SAMPLING DATA FROM PLANT 12036.  .

V-21      SUMMARY OF SAMPLING DATA FROM PLANT 4086  .  .

V-22      SUMMARY OF SAMPLING DATA FROM PLANT 36070.  .

V-23      SUMMARY OF SAMPLING DATA FROM PLANT 6070  .  .

V-24      SUMMARY OF SAMPLING DATA FROM PLANT 6058  .  .
                                          i

          SUMMARY OF SAMPLING DATA FROM PLANT 6461  .  .
                                                             124

                                                             130

                                                             136

                                                             140

                                                             143

                                                             152

                                                             156

                                                             166
V-25

V-26      METALS REPORTED AS RAW MATERIALS BY COPPER
          AND COPPER ALLOY PRODUCTS PLANTS 	    175

VI-1      POLLUTANTS NOT DETECTED IN COPPER FORMING
          WASTEWATER	    221

VI-2      POLLUTANTS EXCLUDED FROM REGULATION BECAUSE
          THEY ARE PRESENT IN AMOUNTS TOO SMALL TO BE
          EFFECTIVELY TREATED	f	    224

VI-3      POLLUTANTS CONSIDERED FOR REGULATION  	    225

VI-4      MAXIMUM CONCENTRATIONS OF TOXIC!POLLUTANTS
          FOUND IN COPPER FORMING WASTEWATERS	    226

VII-1     pH CONTROL EFFECT ON METALS REMOVAL	    346

VII-2     EFFECTIVENESS OF SODIUM HYDROXIDE FOR METALS
          REMOVAL	    347

VII-3     EFFECTIVENESS OF LIME AND SODIUM HYDROXIDE
          FOR METALS REMOVAL	1	" •    348
                                          i
VII-4     THEORETICAL SOLUBILITIES OF HYDROXIDES  AND
          SULFIDES OF SELECTED METALS IN  PURE WATER.  .  .  .    349

VII-5     SAMPLING DATA FROM SULFIDE PRECiPITATION-
          SEDIMENTATION SYSTEMS	  .  .	    350
                               XXV

-------
                    LIST OF TABLES  (Continued)
Number
Title
Page
VII-6

VII-7
VII-8
VII-9
VII-10
VII-11
VII-12



VII-13
VII-14
VII-15
VII-16
VII-17

VII-18

VII-19

VII-20

VII-21
VII-22

VII-23
SULFIDE PRECIPITATION-SEDIMENTATION
PERFORMANCE. ... 	
FERRITE CO -PRECIPITATION PERFORMANCE 	 	
CONCENTRATION OF TOTAL CYANIDE (mg/1) 	
MULTIMEDIA FILTER PERFORMANCE 	 	
PERFORMANCE OF SELECTED SETTLING SYSTEMS ....
SKIMMING PERFORMANCE . 	 	
SAMPLING DATA FROM COPPER FORMING PLANTS
WHICH PRACTICE OIL SKIMMING AND ACHIEVE
EFFLUENT OIL AND GREASE CONCENTRATIONS OF
20 mg/1 OR LESS 	 	
CHEMICAL EMULSION BREAKING EFFICIENCIES. ....
COMBINED METALS DATA EFFLUENT VALUES (mg/1). . .
L&S PERFORMANCE ADDITIONAL POLLUTANTS 	
COMBINED METALS DATA SET - UNTREATED WASTEWATER.
MAXIMUM POLLUTANT LEVEL IN UNTREATED WASTEWATER
ADDITIONAL POLLUTANTS (mg/1) 	
PRECIPITATION-SETTLING-FILTRATION (LS&F)
PERFORMANCE PLANT A 	 ........
PRECIPITATION-SETTLING-FILTRATION (LS&F)
PERFORMANCE PLANT B 	 	
PRECIPITATION-SETTLING-FILTRATION (LS&F)
PERFORMANCE PLANT C 	 	 	 .
SUMMARY OF TREATMENT EFFECTIVENESS (mg/1). . . .
TREATABILITY RATING OF PRIORITY POLLUTANTS
UTILIZING CARBON ADSORPTION. ... 	 .
CLASSES OF ORGANIC COMPOUNDS ABSORBED ON CARBON. '

351
352
353
354
355
356



357
358
359
360
361

362

363

364

365
366

367
368
                               XV

-------
                     LIST OF TABLES (Continued)


Number         Title                                        Page

VII-24   ACTIVATED CARBON PERFORMANCE .	    369

VII-25   ION EXCHANGE  PERFORMANCE .  .  .  .	    370

VII-26   PEAT ADSORPTION PERFORMANCE.  .	    371

VII-27   MEMBRANE  FILTRATION SYSTEM  EFFLUENT	  .    372

VII-28   ULTRAFILTRATION PERFORMANCE.  ..........    373

VIII-1   CLARIFIER CHEMICAL REQUIREMENTS. '.	    412

VIII-2   CHARACTERISTICS OF THE  COPPER FORMING NORMAL
          PLANT	  .    413

VIII-3   SUMMARY OF COPPER FORMING NORMAL  PLANT COSTS .  .    414

IX-1      BPT FOR HOT ROLLING SPENT LUBRICANT	    424

IX-2      BPT FOR COLD  ROLLING SPENT  LUBRICANT  ......    424

IX-3      BPT FOR DRAWING SPENT LUBRICANT.	  .    425

IX-4      BPT FOR SOLUTION HEAT TREATMENT.	  .    425

IX-5      BPT FOR EXTRUSION HEAT  TREATMENT	  .    426

IX-6      BPT FOR ANNEALING WITH  WATER  .	  .    426

IX-7      BPT FOR ANNEALING WITH  OIL  ...!.'	    427
                                           t
IX-8      BPT FOR ALKALINE CLEANING RINSE.	    427

IX-9      BPT FOR ALKALINE CLEANING BATH	    428

IX-10     BPT FOR PICKLING RINSE	    428

IX-11     BPT FOR PICKLING BATH	    429

IX-12     BPT FOR PICKLING FUME SCRUBBER	    429

X-l       BAT REGULATORY  FLOWS  FOR  COPPER FORMING
          WASTE STREAMS REQUIRING FLOW REDUCTION 	    443

X-2       BAT  FOR HOT ROLLING  SPENT LUBRICANT	    444
                               xvi

-------
                    LIST OF TABLES  (Continued)






Number         Title                                        Page



X-3       BAT FOR COLD ROLLING SPENT LUBRICANT	   444.



X-4       BAT FOR DRAWING SPENT LUBRICANT	   445



X-5       BAT FOR SOLUTION HEAT TREATMENT	   445




X-6       BAT FOR EXTRUSION HEAT TREATMENT	   446



X-7       BAT FOR ANNEALING WITH WATER	   446




X-8       ,BAT FOR ANNEALING WITH OIL	   447




X-9       BAT FOR ALKALINE CLEANING RINSE.	   447



X-10    .  BAT FOR ALKALINE CLEANING BATH	   448




X-ll      BAT FOR PICKLING RINSE	   448




X-12      BAT FOR PICKLING BATH	.	   449



X-13      BAT FOR PICKLING FUME SCRUBBER	   449



XI-1      NSPS FOR HOT ROLLING SPENT LUBRICANT	   455




XI-2      NSPS FOR COLD ROLLING SPENT LUBRICANT	   455



XI-3      NSPS FOR DRAWING SPENT LUBRICANT	   456



XI-4      NSPS FOR SOLUTION HEAT TREATMENT	   456




XI-5      NSPS FOR EXTRUSION HEAT TREATMENT.  .	   457



XI-6 ,     NSPS FOR ANNEALING WITH WATER.	   457



XI-7      NSPS FOR ANNEALING WITH OIL	   458




XI-8      NSPS FOR ALKALINE CLEANING RINSE	   458



XI-9      NSPS FOR ALKALINE CLEANING BATH	   459



XI-10     NSPS FOR PICKLING RINSE.	   459



XI-11     NSPS FOR PICKLING BATH	   460



XI-12     NSPS FOR PICKLING FUME SCRUBBER	   460
                              xvii

-------
                    LIST OF TABLES  (Continued)
Number
XII-1

XII-2
XII-3
XII-4
XII-5
XII-6
XII-7
XII-8
XII-9
XII-10
XII-11
XII-12
XII-13
XII-14
XII-15
XII-16
XII-17
XII-18
XII-19
XII-20
XII-21
XII-22
     Title
TOXIC ORGANIC POLLUTANTS SELECTED FOR REGULATION
FOR COPPER FORMING INDIRECT DISCHARGERS	
PSES FOR HOT ROLLING SPENT LUBRICANT  .
PSES FOR COLD ROLLING SPENT LUBRICANT.
PSES FOR DRAWING SPENT LUBRICANT  .  .  .
PSES FOR SOLUTION HEAT TREATMENT  .  .  .
PSES FOR EXTRUSION HEAT TREATMENT.  .  .
PSES FOR ANNEALING WITH WATER	
PSES FOR ANNEALING WITH OIL. .  .  .  .  ,
PSES FOR ALKALINE CLEANING RINSE ;.  .  ,
PSES FOR ALKALINE CLEANING BATH.  .  .  .
PSES FOR PICKLING RINSE	;.  .  ,
PSES FOR PICKLING BATH	
PSES FOR PICKLING FUME SCRUBBER.  .  .  ,
PSNS FOR HOT ROLLING SPENT LUBRICANT  ,
PSNS FOR COLD ROLLING SPENT LUBRICANT,
PSNS FOR DRAWING SPENT LUBRICANT  .  .
PSNS FOR SOLUTION HEAT TREATMENT  .  .
PSNS FOR EXTRUSION HEAT TREATMENT.  .
PSNS FOR ANNEALING WITH WATER.  ...
PSNS FOR ANNEALING WITH OIL. ....
PSNS FOR ALKALINE CLEANING RINSE  .  .
                                 i
PSNS FOR ALKALINE CLEANING BATH.  .  .
467
468
468
469
469
470
470
471
471
472
472
473
473
474
474
475
475
476
476
477
477
478
                               xviii

-------
                    LIST OF TABLES  (Continued)






Number         Title



XII-23    PSNS FOR PICKLING RINSE	



XII-24    PSNS FOR PICKLING BATH 	




XII-25    PSNS FOR PICKLING FUME SCRUBBER.  .  .
Page



 478



 479



 479
                               X1.X

-------
XX

-------
                             SECTION I

                      SUMMARY AND  CONCLUSIONS
Pursuant to Sections  301,  304,  306,  307,  and 501  of the  Clean
Water Act and  the provisions  of the  Settlement  Agreement in
Natural Resources Defense  Council v.  Train,  8 ERG 2120 (D.D.C.
1976) modified,  12 ERG  1833  (D.D.C.  1979),  EPA  has  collected and
analyzed data "for plants in the Copper  Forming  Point Source
Category.  EPA has never proposed or promulgated  effluent limita-
tions or standards for  this industry. This  document and  the
administrative record provide the technical  basis for proposing
effluent limitations based on best practicable  technology (BPT)
and best available technology (BAT)  for existing  direct  dis-
chargers, pretreatment  standards for existing indirect dis-
chargers (PSES), pretreatment standards for  new indirect
dischargers (PSNS), and standards of performance  for new source
direct dischargers (NSPS).

The copper forming category is  comprised  of  176 plants.   Of the
176 plants, 37 discharge directly to rivers,  lakes,  or streams;
45 discharge to  publicly owned  treatment  works  (POTW); and  94
achieve zero discharge of  process wastewater.

EPA first studied the Copper  Forming Point Source Category  to
determine whether differences in raw materials, final  products,
manufacturing  processes, equipment,  age and  size  of plants,  water
usage, required  the development  of separate  effluent limitations
and standards  for different segments  of the  category.  This
involved a detailed analysis  of wastewater discharge and treated
effluent characteristics,  including  (1) the  sources  and  volume  of
water used, the  processes  employed,  and the  sources  of pollutants
and wastewaters  in the plant; and (2) the constituents of waste-
waters, including toxic pollutants.

EPA also identified several distinct  control  and  treatment
technologies (both in-plant and end-of-pipe)  applicable  to  the
Copper Forming Point Source Category.   The Agency analyzed  both
historical and newly generated  data  on  the performance of these
technologies,  including their nonwater  quality  environmental
impacts and air quality, solid waste  generation,  and energy
requirements.  EPA also studied various flow  reduction techniques
reported in the data collection portfolios  (dcp)  and plant
visits.

Engineering costs were prepared for  each of the control  and
treatment options considered  for the  category.  These  costs were
then used by the Agency to estimate  the impact  of implementing
the various options on the industry.  For each  control and

-------
treatment option that the Agency found to be most effective and
technically feasible in controlling the discharge of pollutants,
the number of potential closures, number of employees affected,
and impact on price were estimated.  These results are reported
in a separate document entitled "The Economic Impact Analysis of
Effluent Limitations Guidelines and Standards for the Copper
Forming Industry."
                                           !
Based on consideration of the above factors, EPA identified vari-
ous control and treatment technologies which formed the basis for
BPT and selected control and treatment appropriate for each set
of standards and limiations.  The mass limitations and standards
for BPT, BAT, NSPS, PSES, and PSNS are presented in Section II.

-------
                             SECTION II

                          REG OMMENDATIONS


 This  section presents  the effluent limitations and standards
 which are proposed for the Copper Forming Point Source Category
 for BPT,  BAT,  PSES,  NSPS, and PSNS.   It also presents alternate
 limitations  and standards for BAT and PSES following the proposed
 limitations  and standards.

 BPT

 EPA is  proposing BPT for  copper  forming plants based on the
 treatment effectiveness achieved by  the application of chemical
 precipitation  and sedimentation  (lime and settle)  technology and,
 where_required,  preliminary treatment consisting of chemical
 emulsion  breaking, oil skimming,  and hexavalent chromium reduc-
 tion.   The following BPT  effluent limitations  are  being proposed
 for existing sources:
 (a)  BPT FOR HOT ROLLING  SPENT LUBRICANT
Pollutant or Pollutant Property
          Maximum
          For Any
          One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
      Milligrams Per Off Kilogram
(Ibs/million Ibs) of Copper Hot Rolled

             0.044         0.018
             0.20          0.11
             0.016         0.014
             0.15          0.11
             0.14          0.06
             2.06          1.24
             4.23          2.06
    Within  the  range of 7.5 to 10.0
              at all  times

-------
(b)  BPT FOR COLD ROLLING SPENT "LUBRICANT
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Average
                               Milligrams Per Off Kilogram
                         (Ibs/million Ibs) of Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
        0.16
      0.065
        0.72          0.38
        0.057         0.050
        0.54          0.38
        0.51          0.22
        7.58          4.55
       15.54          7.58
Within the range of 7.5 to 10.0
         at all times
(c)  BPT FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
        0
        0
        0
        0
        0
        0
        0
      0
      0
      0
      0
      0
      0
      0

-------
 (d)   BPT  FOR SOLUTION  HEAT  TREATMENT
 Pollutant  or Pollutant Property
            Maximum
            For Any
            One Day
  Maximum  for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
PH
                                  Milligrams Per Off Kilogram
                                        (Ibs/million Ibs)
                                  of Copper Quenched in Water
               1.07
               4.83
               0.39
               3.58
               3.38
              50.82
             104.19
      0.43
      2.54
      0.33
      2.54
      1.42
     30.49
     50.82
       Within the range of 7.5 to 10.0
                at all times
 (e)  BPT FOR EXTRUSION HEAT TREATMENT
Pollutant or Pollutant Property
            Maximum
            For Any
            One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
       Milligrams  Per Off Kilogram
(Ibs/million Ibs)  of Copper Heat Treated
         on an Extrusion Press

               0.00084      0.00034
               0.0038       0.0020
               0.00030      0.00026
               0.0028       0.0020
               0.0026       0.0011
               0.040        0.024
               0.082        0.040
       Within the  range  of  7.5 to 10.0
               at all times

-------
(£)  BPT FOR ANNEALING WITH WATER
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                            (Ibs/million Ibs)  of Copper Annealed
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
        2.38
       10.77
        0.85
        7.99
        7.54
      113.34
      232.35
      0.97
      5.67
      0.74
      5.67
      3.17
     68.00
    113.34
Within the range of-7.5 to 10.0
         at all times
 (g)  BPT FOR ANNEALING WITH OIL
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                            (Ibs/million Ibs) of Copper Annealed
                                and Quenched in a Lubricant
                                         Solution
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
PH
        0
        0
        0
        0
        0
        0
        0
      0
      0
      0
      0
      0
      0
      0
Within the range of 7.5 to 10.0
         at all times

-------
 (h)  BPT FOR ALKALINE CLEANING RINSE
 Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
   Maximum for
 Monthly Averae
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 Oil  and Grease
 TSS
 PH
    Milligrams Per Off Kilogram
    (Ibs/million Ibs)  of Copper
         Alkaline Cleaned

         1.77           0.72
         8.01           4.21
         0.63           0.55
         5.94           4.21
         5.60           2.36
        84.28          50.57
       172.77          84.28
Within the range  of 7.5  to 10.0
          at all times
 (i)   BPT FOR ALKALINE CLEANING BATH
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Averat
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
   Milligrams Per Off Kilogram
   (Ibs/million Ibs) of Copper
        Alkaline Cleaned

        0.020         0.0080
        0.089         0.047
        0.0071        0.0061
        0.066         0.047
        0.062         0.026
        0.93          0.56
        1.91          0.94
Within the range of 7.5 to 10.0
         at all times

-------
(j)  BPT FOR PICKLING RINSE
Pollutant or Pollutant Property
    Maximum
    For Any
    One Day
                  Maximum for
                Monthly Average
                                 Milligrams Per Off Kilogram
                             (Ibs/million Ibs)  of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
PH
                                         52
        1.
        6.88
        0.54
        5.12
        4.82
       72.44
      148.50
Within the range of 7.5 to 10.0
         at all times
                     0.62
                     3.62
                     0.47
                     3.62
                     2.03
                    43.46
                    72.44
 (k)  BPT FOR PICKLING BATH
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
                  Maximum for
                Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of.Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
                                       0.049
                      0.020
        0.22          0.12
        0.017         0.015
        0.16          0.12  '
        0.16          0.065
        2.32          1.39
        4.76          2.32
Within the range of 7.5 to  10.0
         at all times

-------
 (1)  BPT FOR PICKLING FUME  SCRUBBER
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum  for
Monthly Average
                                 Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
        0.26
        1.19
        0.094
        0.88
        0.83
       12.52
       25.67
      0.11
      0.63
      0.081
      0.63
      0.35
      7.51
     12.52
Within the range of 7.5 to 10.0
         at all times
BAT

EPA is proposing BAT for copper forming plants based on treatment
effectiveness achieved through reduction of water discharge from
solution heat treatment and annealing water by recycle, pickling
rinse by implementing spray rinsing with recirculation, and by
end-of-pipe treatment consisting of oil skimming, chemical
precipitation and sedimentation and, where required, preliminary
treatment with chemical emulsion, oil skimming and hexavalent
chromium reduction.  The following BAT limitations are being.
proposed for existing sources:
(a)  BAT FOR HOT ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
     Maximum
     For Any
     One Day
  Maximum for
Monthly Average
                               Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Hot Rolled
Chromium
Copper
Lead
Nickel
Zinc
        0.044
        0.20
        0.016
        0.15
        0.14
      0.018
      0.11
      0.014
      0.11
      0.058

-------
(b)  BAT FOR COLD ROLLING SPENT LUBRICANT
Pollutant, or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                              Milligrams Per Off Kilogram
                         (Ibs/million Ibs)iof Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
   0.16
   0.72
   0.057
   0.54
   0.51
      0.065
      0.38
      0.050
      0.38
      0.22
(c)  BAT FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
(d)  BAT FOR SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                                  (Ibs/million Ibs) of Copper
                                       Quenched in Water
Chromium
Copper
Lead
Nickel
Zinc
   0.27
   1.23
   0.097
   0.91
   0.86
      0.11
      0.65
      0.084
      0.65
      0.36
                               10

-------
(e)  BAT FOR EXTRUSION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams  Per Off Kilogram
                                  (Ibs/million  Ibs)  of  Copper
                                  Extruded and  Quenched in  a
                                      Lubricant Solution
Chromium
Copper
Lead
Nickel
Zinc
(f) BAT FOR ANNEALING WITH WATER
Pollutant or Pollutant Property

Chromium
Copper
Lead
Nickel
Zinc
(g) BAT FOR ANNEALING WITH OIL
Pollutant or Pollutant Property
0.00084
0.0038
0.00030
0.0028
0.0026

Maximum
For Any
One Day
0.00034
0.0020
0.00026
0.0020
0.0012

Maximum for
Monthly Average
Milligrams Per Off Kilogram
(Ibs/million Ibs) of Copper
Annealed and Quenched in Water
0.52
2.36
0.19
1.75
1.65

Maximum
For Any
One Day
0.21
1.24
0.16
1.24
0.69

Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                                  (Ibs/million Ibs) of Copper
                                  Annealed and Quenched in a
                                      Lubricant Solution
Chromium
Copper
Lead
Nickel
Zinc
    0
    0
    0
    0
    0
       0
       0
       0
       0
       0
                               11

-------
 (h)  BAT FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
                                  Milligrams Per Off Kilogram
                                  (Ibs/million Ibs) of Copper
                                       Alkaline Cleaned
   1.77
   8.01
   0.63
   5.94
   5.60
      0.72
      4.21
      0.55
      4.21
      2.36
 (i)  BAT FOR ALKALINE CLEANING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
                                  Milligrams Per Off Kilogram
                                  (Ibs/million Ibs) of Copper
                                       Alkaline Cleaned
   0.020
   0.089
   0.0071
   0.066
   0.062
      0.0080
      0.047
      0.0061
      0.047
      0.026
(j)  BAT FOR PICKLING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
   0.55
   2.48
   0.20
   1.84
   1.74
      0.22
      1.31
      0.17
      1.31
      0.73
                               12,

-------
(k)  BAT FOR PICKLING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
   0.049
   0.22
   0.017
   0.16
   0.15
      0.020
      0.12
      0.015
      0.12
      0.06
(1)  BAT FOR PICKLING FUME SCRUBBER
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
   0.26
   1.19
   0.094
   0.88
   0.83
      0.11
      0.63
      0.081
      0.63
      0.35
NSPS

EPA is proposing NSPS for copper forming plants based on treat-
ment effectiveness used for BAT with the addition of end-of-pipe
filtration and the reduction of pickling rinse water flow based
on the use of countercurrent rinsing.  The following standards
are being proposed for new sources:
                               13

-------
 (a)  NSPS  FOR HOT ROLLING  SPENT LUBRICANT
 Pollutant  or Pollutant Property
          Maximum
          For Any
          One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
    .  Milligrams Per Off Kilogram
(Ibs/million  Ibs)  of Copper Hot Rolled

             0.038        0.016
             0.13          0.063
             0.011        0.0093
             0.057        0.038
             0.11          0.043
             1.03          1.03
             1.55          1.13
    Within the range of 7.5 to 10.0
             at ail times
 (b)  NSPS FOR COLD ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
         Maximum
         For Any
         One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Cold Rolled
Chromium     •
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
PH
            0.14
            0.49
            0.038
            0.21
            0.39
            3.79
            5.69
      0.057
      0.23
      0.034
      0.14
      0.16
      3.79
      5.07
    Within the range of 7.5 to 10.0
             at all times
                              14

-------
(c)  NSPS FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
     Maximum
    .For Any
     One Day
    Maximum for
:  Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
        0
        0
        0
        0
        0
        0
        0
        0
        0
        0
        0
        0
        0
        0
Within the range of 7.5 to 10.0
         at all times
 (d)  NSPS FOR SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
     Maximum
     For Any
     6ne Day
 ,.  Maximum for
  Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Quenched
                                            in Water
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
        0.24
        0.83
        0.065
        0.36
        0.66
        6.46
        9.69
        0.097
        0.39
        0.058
        0.24
        0.27
        6.46
        7.11
Within the range of 7.5 to 10.0
         at all times
                               15

-------
 (e)  NSPS FOR EXTRUSION HEAT TREATMENT
Pollutant or Pollutant Property
        Maximum
        For Any
        One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
    Milligrams Per Off Kilogram
(Ibs/million  Ibs)  of Copper Extruded
        and Quenched in Oil

          0.00074       0.00030
          0.0026         0.0012
          0.00020       0.00018
          0.0011         0.00074
          0.0021         0.00084
          0.020          0.020
          0.030          0.022
  Within  the range of 7.5 to 10.0
           at all times
 (f)  NSPS FOR ANNEALING WITH WATER
Pollutant or Pollutant Property
       Maximum
       For Any
       One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
     Milligrams Per Off Kilogram
 (Ibs/million Ibs) of Copper Annealed
        and Quenched in Water

          0.46          0.19
          1.59          0.76
          0.13          0.12
          0.68          0.46
          1.27          0.52
         12.40         12.40
         18.60         13.64
  Within the range of 7.5 to 10.0
           at all times
                               16

-------
(g)  NSPS FOR ANNEALING WITH OIL
Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs)  of Copper Annealed
                                  and Quenched  in a Lubricant
                                           Solution
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
         0
         0
         0
         0
         0
         0
         0
      0
      0
      0
      0
      0
      0
      0
  Within  the  range  of 7.5 to 10.0
           at all times
 (h)  NSPS FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
     Milligrams Per Off Kilogram
(Ibs/million  Ibs)  of  Copper Alkaline
              Cleaned

          1.56          0.63
          5.39          2.57
          0.42          0.38
          2.32          1.56
          4.30          1.77
         42.14         42.14
         63.21         46.35
  Within the  range of 7.5  to  10.0
           at all  times
                                17

-------
          (i)  NSPS FOR ALKALINE CLEANING BATH
          Pollutant or Pollutant Property
       Maximum
       For Any
       One Day
  Maximum for
Monthly Average
          Chromium
          Copper
          Lead
          Nickel
          Zinc
          Oil and Grease
          TSS
          pH
     Milligrams Per Off Kilogram
(Ibs/million  ibs)  of Copper Alkaline
              Cleaned

          0.017         0.0070
          0.060         0.029
          0.0047        0.0042
          0.026         0.017
          0.048         0.020
          0.47          0.47
          0.70       ,  0.51
  Within  the  range of 7.5 to 10.0
           at all  times
          (j)  NSPS FOR PICKLING RINSE
          Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
  Maximum for
Monthly Average
                                            Milligrams Per Off Kilogram
                                        (Ibs/million Ibs) of Copper Pickled
          Chromium
          Copper
          Lead
          Nickel
          Zinc
          Oil and Grease
          TSS
          pH
          0.22
          0.75
          0.059
          0.32
          0.60
          5.85
          8.78
      0.088
      0.36
      0.053
      0.22
      0.25
      5.85
      6.44
 Within  the range of 7.5 to 10.0
           at  all times
                                         18
_

-------
(k)  NSPS FOR PICKLING BATH
Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
    Milligrams  Per Off Kilogram
(Ibs/million Ibs)  of Copper Pickled

         0.043         0.018
         0.15         0.071
         0.012         0.011
         0.065         0.043
         0.12         0.048
         1.16         1.16
         1.74         1.28
 Within the range  of 7.5  to 10.0   '..
          at all times
(1)  NSPS FOR PICKLING FUME SCRUBBER
Pollutant or Pollutant Property
      Maximum
      For Any
      One Day
  Maximum for
Monthly Average
Chromium
Copper
Lead
Nickel
Zinc
Oil and Grease
TSS
pH
    Milligrams Per Off Kilogram
(Ibs/million Ibs)  of Copper Pickled

         0.23          0.094
         0.81          0.38
         0.063         0.057
         0.35          0.23
         0.64          0.26
         6.26          6.26
         9.39          6.89
 Within the range  of 7.5 to 10.0
          at all times
                               19

-------
PSES                                       ;

EPA is proposing PSES for copper forming plants based on treat-
ment effectiveness used for BAT.  The following standards are
being proposed for existing sources:
 (a)  PSES FOR HOT ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Hot Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease (for alternate
  monitoring)
   0.044
   0.20
   0.016
   0.15
   0.14
   0.032
   2.06
      0.018
      0.11
      0.014
      0.11
      0.058
      0.025
      1.24
(b)  PSES FOR COLD ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0.16
   0.72
   0.057
   0.54
   0.51
   0.12
   7.58
      0.065
      0.38
      0.050
      0.38
      0.22
      0.091
      4.55
                               20

-------
(c)  PSES FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
      0
(d)  PSES FOR SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) o£ Copper Quenched
                                           in Water
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0.27
   1.23
   0.097
   0.91
   0.86
   0.20
  12.92
      0.11
      0.65
      0.084
      0.65
      0.36
      0.16
      7.75
                               21

-------
          (e)   PSES FOR EXTRUSION HEAT TREATMENT
          Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                            Milligrams  Per Off Kilogram
                                       (Ibs/million Ibs)  of Copper Extruded
                                            and Quenched  in a Lubricant
                                                     Solution
          Chromium
          Copper
          Lead
          Nickel
          Zinc
          TTO
          Oil EC Grease (for alternate
            monitoring)
   0.00084
   0.0038
   0.00030
   0.0028
   0.0027
   0.00062
   0.040
      0.00034
      0.0020
      0.00026
      0.0020
      0.0012
      0.00048
      0.024
          (f)  PSES FOR ANNEALING WITH WATER
          Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                            Milligrams Per Off Kilogram
                                       (Ibs/million Ibs)  of Copper Annealed
                                               and Quenched in Water
          Chromium
          Copper
          Lead
          Nickel
          Zinc
          TTO
          Oil 8c Grease (for alternate
            monitoring)
   0.52
   2.36
   0.19
   1.75
   1.65
   0.38
  24.80
      0.21
      1.24
      0.16
      1.24
      0.70
      0.30
     14.88
                                         22
-

-------
 (g)  PSES FOP. ANNEALING WITH OIL
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Annealed
                                  and Quenched in a Lubricant
                                           Solution
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease (for alternate
  monitoring)
   0
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
      0
(h)  PSES FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil St Grease (for alternate
  monitoring)
   1.77
   8.01
   0.63
   5.94
   5.60
   1.31
  84.28
      0.72
      4.21
      0.55
      4.21
      2.36
      1.01
     50.57
                               23

-------
(t)  PSES FOR ALKALINE CLEANING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs)  of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0.020
   0.089
   0.0071
   0.066
   0.062
   0.014
   0.93
      0.0080
      0.047
      0.0061
      0.047
      0.026
      0.011
      0.56
 (j)  PSES FOR PICKLING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum  for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Pickled
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 TTO
 Oil Sc Grease (for alternate
   monitoring)
    0.55
    2.48
    0.20
    1.84
    1.74
    0.41
   26.12
       0.22
       1.31
       0.17
       1.31
       0.73
       0.31
      15.67
                                24

-------
(k)  PSES FOR PICKLING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil 8t Grease (for alternate
  monitoring)
   0.049
   0.22
   0.018
   0.17
   0.16
   0.036
   2:32
      0.020
      0.12
      0.015
      0.12
      0.065
      0.028
      1.39
(1)  PSES FOR PICKLING FUME SCRUBBER
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Lead
Nickel
Copper
Zinc
TTO
Oil St Grease (for alternate
  monitoring)
   0.26
   1.19
   0.094
   0.88
   0.83
   0.19
  12.51
      0.11
      0.63
      0.082
      0.63
      0.35
      0.15
      7.51
                               25

-------
PSNS

EPA is proposing PSNS for copper forming plants based on treat-
ment effectiveness for NSPS.  The following standards are being
proposed for new sources:
(a)  PSNS FOR HOT ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Hot Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0.038
   0.13
   0.011
   0.057
   0.11
   0.022
   1.03
      0.016
      0.063
      0.0093
      0.038
      0.043
      0.022
      1.03
(b)  PSNS FOR COLD ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum'
For Any
One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                          (Ibs/million Ibs) of Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease  (for alternate
  monitoring)
   0.14
   0.49
   0.038
   0.2l
   0.39
   0.080
   3.79
      0.057
      0.23
      0.034
      0.14
      0.16
      0.080
      3.79
                                26

-------
(c)  PSNS FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
      0
 (d)  PSNS FOR SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Quenched
                                            in Water
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease  (for alternate
  monitoring)
   0.24
   0.83
   0.065
   0.36
   0.66
   0.14
   6.46
      0.097
      0.39
      0.058
      0.24
      0.27
      0.14
      6.46
                               27

-------
 (e)  PSNS FOR EXTRUSION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Extruded
                                 and Quenched in a Lubricant
                                          Solution
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Se Grease  (for alternate
  monitoring)
   0.00074
   0.0026
   0.00020
   0.0011
   0.0021
   0.00042
   0.020
      0.00030
      0.0013
      0.00018
      0.00074
      0.00084
      0.00042
      0.020
 (f)  PSNS FOR ANNEALING WITH WATER
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Annealed
                                    and Quenched in Water
Chromium
Copper
-Lead
Nickel
Zinc
TTO
Oil Sc Grease  (for alternate
  monitoring)
   0.46
   1.59
   0.13
   0.68
   1.27
   0.26
  12.40
      0.19
      0.76
      0.12
      0.46
      0.52
      0.26
     12.40
                               28

-------
(g)  PSNS FOR ANNEALING WITH OIL
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                             (Ibs/million Ibs)  of Copper Annealed
                                 and Quenched in a Lubricant
                                          Solution
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
      0
 (h)  PSNS FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 TTO
 Oil Sc Grease (for  alternate
   monitoring)
    1.56
    5.39
    0.42
    2.32
    4.30
    0.89
   42.14
       0.63
       2.57
       0.38
       1.56
       1.77
       0.89
      42.14
                                29

-------
 (i)   PSNS  FOR ALKALINE CLEANING  BATH
 Pollutant  or  Pollutant Property
Maximum
For Any
One Day
  Maximum  for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil St Grease  (for alternate
  monitoring)
   0.017
   0.060
   0.0047
   0.026
   0.048
   0.0099
   0.47
      0.0070
      0.029
      0.0042
      0.017
      0.020
      0.0099
      0.47
 (j)  PSNS FOR PICKLING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease (for alternate
  monitoring)
   0.22
   0.75
   0.059
   0.32
   0.60
   0.12
   5.85
      0.088
      0.36
      0.053
      0.22
      0.25
      0.12
      5.85
                              30

-------
(k)  PSNS FOR PICKLING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil & Grease (for alternate
  monitoring)
   0.043
   0.15
   0.012
   0.064
   0.12
   0.024
   1.16
      0.018
      0.071
      0.011
      0.043
      0.048
      0.024
      1.16
 (1)  PSNS FOR PICKLING FUME SCRUBBER
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
TTO
Oil Sc Grease  (for alternate
  monitoring)
   0.23
   0.81
   0.063
   0.35
   0.64
   0.13
   6.26
      0.094
      0.38
      0.057
      0.23
      0.26
      0.13
      6.26
ALTERNATE BAT AND PSES

EPA  is  considering promulgating BAT effluent limitations more
stringent than the limitations now proposed for BAT.  The
limitations  are based upon  the treatment effectiveness achieved
through the  control and treatment used to form the basis of BAT,
with the addition of filtration.  In the event that the Agency
decides to promulgate these more stringent limitations, the
following would apply:
                                31

-------
(a)  BAT FOR HOT ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                           (Ibs/million Ibs) of Copper Hot Rolled
Chromium
Copper
Lead
Nickel
Zinc
   0.038
   0.13
   0.010
   0.057
   0.11
      0.010
      0.050
      0.0082
      0.030
      0.032
(b)  BAT FOR COLD ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams Per Off Kilogram
                          (Ibs/million Ibs;) of Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
   0.14
   0.49
   0.038
   0.21
   0.39
      0.038
      0.19
      0.030
      0.11
      0.12
(c)  BAT FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                                (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
                                32

-------
(d)  BAT FOR SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Quenched
                                           in Water
Chromium
Copper
Lead
Nickel
Zinc
   0.24
   0.83
   0.065
   0.36
   0.66
      0.065
      0.32
      0.052
      0.19
      0.20
(e)  BAT FOR EXTRUSION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum  for
Monthly Average
                                  Milligrams  Per  Off  Kilogram
                              (Ibs/million  Ibs)  of Copper  Extruded
                                  and  Quenched  in a Lubricant
                                            Solution
Chromium
Copper
Lead
Nickel
Zinc
    0.00074
    0.0026
    0.00020
    0.0011
    0.0020
       0.00020
       0.00098
       0.00016
       0.00058
       0.00062
 (f)  BAT FOR ANNEALING WITH WATER
 Pollutant  or Pollutant  Property
 Maximum
 For  Any
 One  Day
  Maximum for
Monthly Average^
                                   Milligrams Per Off Kilogram
                              (Ibs/million Ibs)  of Copper Annealed
                                      and Quenched in Water
 Chromium
 Copper
 Lead
 Nickel
 Zinc
    0.46
    1.59
    0.12
    0.68
    1.26
       0.12
       0.61
       0.099
       0.36
       0.38
                                33

-------
 (g)   BAT  FOR ANNEALING WITH OIL
Pollutant  or  Pollutant  Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams  Per  Off  Kilogram
                              (Ibs/million  Ibs)  of Copper Annealed
                                  and  Quenched  in a Lubricant
                                           ! Solution
Chromium
Copper
Lead
Nickel
Zinc
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
 (h)  BAT FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
   1.56
   5.39
   0.42
   2.32
   4.30
      0.42
      2.06
      0.34
      1.22
      1.31
(i)  BAT FOR ALKALINE CLEANING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
   0.017
   0.060
   0.0047
   0.026
   0.048
      0.0047
      0.023
      0.0037
      0.014
      0.014
                               34

-------
(j)  BAT FOR PICKLING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
   0.48
   1.67
   0.13
   0.72
   1.33
      0.13
      0.64
      0.10
      0.38
      0.40
 (k)  BAT FOR PICKLING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum  for
Monthly Average
                                  Milligrams  Per  Off  Kilogram
                               (Ibs/million  Ibs) of  Copper  Pickled
 Chromium
 Copper
 Lead
 Nickel
 Zinc
    0.043
    0.15
    0.012
    0.064
    0.12
       0.012
       0.057
       0.0093
       0.034
       0.036
 (1)   BAT FOR PICKLING FUME SCRUBBER
 Pollutant or Pollutant Property
 Maximum
 For Any
 One Day
   Maximum for
 Monthly Average
                                   Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Pickled
 Chromium
 Copper
 Lead
 Nickel
 Zinc
    0.23
    0.80
    0.063
    0.34
    0.64
       0.063
       0.31
       0.050
       0.18
       0.19
                                35

-------
PSES  (Alternate)

EPA is  considering promulgating PSES  effluent limitations more
stringent  than the limitations  now proposed for PSES.   The
limitations  are based upon the  treatment effectiveness achieved
through the  control and  treatment  used to form the basis  of PSES,
with  the addition of filtration.   In  the event that the Agency
decides to promulgate these more  stringent limitations, the
following  would apply:
 (a)  PSES FOR HOT ROLLING SPENT  LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                 Milligrams  Per  Off Kilogram
                            (Ibs/million  Ibs)  of  Copper  Hot  Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0.038
   0.13
   0.010
   0.057
   0.11
   0.052
      0.010
      0.050
      0.0083
      0.030
      0.032
      0.034
(b)  PSES FOR'COLD ROLLING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                Milligrams Per Off Kilogram
                           (Ibs/million Ibs) of Copper Cold Rolled
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0.14
   0.49
   0.038
   0.21
   0.39
   0.19
      0.038
      0.19
      0.030
      0.11
      0.12
      0.13
                                36

-------
(c)  PSES FOR DRAWING SPENT LUBRICANT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Drawn
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
(d)  PSES FOR. SOLUTION HEAT TREATMENT
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams  Per  Off  Kilogram
                              (Ibs/million  Ibs)  of Copper  Quenched
                                            in Water
Chromium
Copper
Lead
Nickel
Zinc
TTO
    0.24
    0.83
    0.065
    0.36
    0.66
    0.32
       0.065
       0.32
       0.052
       0.19
       0.20
       0.21
 (e)   PSES FOR EXTRUSION HEAT  TREATMENT
 Pollutant  or Pollutant Property
 Maximum
 For Any
 One Day
   Maximum for
 Monthly Average
                                   Milligrams Per Off Kilogram
                                   (Ibs/million Ibs)  of Copper
                                   Extruded and Quenched in a
                                       Lubricant Solution
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 TTO
    0.00074
    0.0026
    0.00020
    0.0011
    0.0020
    0.001
       0.00020
       0.00098
       0.00016
       0.00058
       0.00062
       0.00064
                                37

-------
 (f)  PSES  FOR ANNEALING WITH WATER
Pollutant  or Pollutant  Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams  Per  Off Kilogram
                              (Ibs/million  Ibs)  of Copper  Annealed
                                      and Quenched in Water
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0.46
   1.59
   0.12
   0.68
   1.26
   0.62
      0.12
      0.61
      0.099
      0.36
      0.38
      0.41
 (g)  PSES FOR ANNEALING WITH OIL
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                              (Ibs/million  Ibs) of Copper Annealed
                                  a*nd Quenched in a Lubricant
                                            Solution
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0
   0
   0
   0
   0
   0
      0
      0
      0
      0
      0
      0
(h)  PSES FOR ALKALINE CLEANING RINSE
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
TTO
   1.56
   5.39
   0.42
   2.32
   4.30
   2.11
      0.34
      2.06
      0.34
      0.42
      1.31
      1.39
                               38

-------
(i)  PSES FOR ALKALINE CLEANING BATH
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                             (Ibs/million Ibs) of Copper Alkaline
                                            Cleaned
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0.017
   0.060
   0.0047
   0.026
   0.048
   0.023
      0.0047
      0.023
      0.0037
      0.014
      0.014
      0.015
 (j)  PSES FOR PICKLING RINSE
Pollutant  or Pollutant  Property
Maximum
For Any
One Day
  Maximum  for
Monthly Average
                                  Milligrams  Per Off Kilogram
                               (Ibs/million Ibs)  of Copper Pickled
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 TTO
    0.48
    1.67
    0.13
    0.72
    1.33
    0.65
       0.13
       0.64
       0.10
       0.38
       0.40
       0.43
 (k)   PSES FOR PICKLING BATH
 Pollutant or Pollutant Property
 Maximum
 For Any
 One Day
   Maximum for
 Monthly Average
                                   Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Pickled
 Chromium
 Copper
 Lead
 Nickel
 Zinc
 TTO
    0.043
    0.15
    0.012
    0.064
    0.12
    0.058
       0.012
       0.057
       0.0093
       0.034
       0.036
       0.038
                                39

-------
 (1)  PSES FOR PICKLING FUME SCRUBBER
Pollutant or Pollutant Property
Maximum
For Any
One Day
  Maximum for
Monthly Average
                                  Milligrams Per Off Kilogram
                               (Ibs/million Ibs) of Copper Pickled
Chromium
Copper
Lead
Nickel
Zinc
TTO
   0.23
   0.80
   0.063
   0.34
   0.64
   0.31
      0.063
      0.31
      0.050
      0.18
      0.19
      0.21
                              40

-------
SECTION III

INTRODUCTION
                                    It
The purpose of this document is to present the findings of the
EPA study of the Copper Forming Point Source Category.  The docu-
ment (1) explains which segments of the industry are regulated;
(2) discusses the reasons; and  (3) explains how the actual limi-
tations were developed.  Section I presents a summary of EPA  s
study of the copper forming industry.  Section II presents the
effluent limitations and standards which EPA is proposing for
copper forming wastewaters at BPT, BAT, NSPS, PSES, and PSNS.
also includes limitations and standards based on technology
options which the Agency is continuing to consider  for BAT and
PSES.

Industry data gathered under the authority of Section 308 of  the
Clean Water Act are used throughout this report in  support of
regulating pollutants or excluding pollutants from  regulation
under Paragraph 8 of the Settlement Agreement.  Telephone con-
tacts, literature, and plant visits provided the_information  used
to characterize the industry as detailed in Section III.

Water use and wastewater characteristics in the copper  forming
category are described in Section V in terms of flow and pollu-
tant concentration.  Pollutants excluded from regulation or
selected for consideration are  found  in Section VI.  The dis-
cussion in that section identifies and describes the pollutants
to be regulated and presents the rationale  for regulation or
exclusion.  Section VII describes treatment technology  applicable
to this category and the performance  of these technologies.
Section VIII estimates the capital and operating costs  for  the
treatment technologies used as  the basis for limitations.   The
regulatory limits  and  the bases for these  limitations and
standards are presented in Sections IX through XII.

LEGAL BACKGROUND

The  Federal Water  Pollution Control Act Amendments  of^1972  estab-
lished  a comprehensive program to  "restore  and maintain the
chemical, physical, and biological  integrity of the Nation  s
waters," Section  101(a).   Section  301(b)(l)(A) set a deadline of
July 1, 1977,  for  existing industrial dischargers  to  achieve
"effluent  limitations  requiring the  application of the  best  prac-
ticable control  technology currently  available"  (BPT).   Section
301(b)(2)(A)  set  a deadline of July  1,  1983,  for  these  dis-
chargers to achieve  "effluent  limitations  requiring the applica-
tion of the best  available  technology economically achievable
 (BAT),  which  will  result  in reasonable  further progress toward
the  national  goal  of  eliminating  the  discharge  of all  pollu-
tants."
     41

-------
 Section 306 required that new industrial direct dischargers com-
 ply with new source performance standards (NSPS),  based on best
 available demonstrated technology.   Sections 307(b)  and (c) of
 the Act required  pretreatment standards for new and  existing
 dischargers to  publicly owned treatment works (POTW).   While the
 requirements for  direct dischargers  were to be incorporated into
 National Pollutants Discharge Elimination System (NPDES) premits
 issued  under Section 402,  the Act made pretreatment  standards
 enforceable directly against dischargers to POTW's (indirect dis-
 chargers).

 Section 401(a)(1)  of the 1972 Act does allow requirements  to be
 set case-by-case.   However,  Congress intended control  require-
 ments to be based,  for the most part,  on regulations promulgated
 by the  Administrator of EPA.   Section 304(b) required  regulations
 that establish  effluent limitations  reflecting the ability of BPT
 and BAT to  reduce  effluent discharge.   Sections 304(c)  and 306 of
 the Act required promulgation of regulations for NSPS.   Sections
 304(f),  307(b), and 307(c) required  regulations for  pretreatment
 standards.   In  addition to these regulations for designated
 industry categories,  Section 307(a)  required the Administrator to
 promulgate  effluent standards applicable to all dischargers of
 toxic pollutants.

 Finally,  Section 501(a)  authorized the Administrator to prescribe
 any additional  regulations "necessary  to carry out his  functions"
 under the Act.                              ,

 The EPA was  unable  to  promulgate many  of these regulations by the
 deadlines contained in the Act,  and  as a result, in  1976,  EPA was
 sued by several environmental groups.   In settling this lawsuit,
 EPA and  the  plaintiffs  executed  a "Settlement Agreement" which
 was approved by the Court.   This agreement  required  EPA to
 develop  a program and  meet a  schedule  for controlling  65 "prior-
 ity" pollutants and classes  of pollutants.   In carrying out this
 program,  EPA must promulgate  BAT effluent limitations guidelines,
 pretreatment standards,  and  new source performance standards for
 21 major  industries.   [See Natural Resources Defense Council,
 Inc. v.  Train,  8 ERG  2120  (D.D.G. 1976),  modified, 12 ERG  1833
 TDTD.C.  1979)].

 Several  of the basic elements  of the Settlement  Agreement  were
 incorporated into the  Clean Water Act  of 19/7.   This law made
 several  important changes  in  the Federal  water pollution control
 program.  Sections  301(b)(2)(A)  and  301(b)(2)(C) of  the Act now
 set July  1,  1984, as the deadline for  industries to  achieve
 effluent  limitations requiring application  of BAT  for "toxic"
 pollutants.   "Toxic" pollutants  here included the  65 "priority"
pollutants and classes  of  pollutants that Congress declared
 "toxic" under Section  307(a)  of  the  Act.
                                42

-------
EPA's programs for new source performance standards and pre-
treatment standards are now aimed principally at controlling
toxic pollutants.  To strengthen the toxics control program,
Section 304(e) of the Act authorizes the Administrator to pre-
sSSe "best management practices"  (BMPs).  These BMPs are  to
prevent the release of toxic and hazardous pollutants from:
P(l) plant site runoff, (2). spillage or  leaks,  (3) sludge or waste
disposal, and  (4) drainage from raw material  storage if any of
these events are associated with, or ancillary  to,  the manufac-
turing or treatment process.

In keeping with its emphasis on toxic pollutants, the Clean Water
Act of 1977 also revises the control program  for non-toxic  pollu-
tants.  For "conventional" pollutants identified under Section
304(a)(4)  (including biochemical oxygen demand, suspended  solids,
fecal coliform, and PH), the new Section 301(b)(2)(E) requires
"effluent  limitations requiring the application of  the best
conventional pollutant control technology"  (BCT)  - instead of
BAT  - to  be achieved by July  1, 1984.   The  factors considered  in
assessing  BCT  for an industry  include the relationship between
the  cost of attaining a reduction  in  effluents  and  the  effluent
reduction  benefits attained, and a  comparison of the cost  and
level of redtiction of such pollutants by publicly owned  treatment
works and  industrial sources.  For  those pollutants that  are
neither  "toxic"  pollutants nor "conventional   pollutants,
Sections 301(b)(2)(A) and  (b)(2)(F) require  achievement  of BAT
effluent limitations within  three  years after their establishment
or July  1,  1984, whichever  is  later,  but not  later than July I,
1987.

The purpose  of this  proposed regulation is  to establish BPT and
BAT effluent  limitations  and NSPS,  PSES, and PSNS for the Copper
Forming  Point  Source Category.

BPT Effluent  Limitations

The factors  considered in defining best practicable control tech-
nology  currently available (BPT)  include:  (1) the total cost of
 applying the technology relative to the effluent reductions that
 result,  (2)  the age of equipment and facilities involved,  (3) the
 processes  used, (4)  engineering aspects of the control technol-
 ogy, (5) process changes, (6) non-water quality environmental
 impacts  (including energy requirements), and  (7) other factors as
 the Administrator considers appropriate.  In general, the  an
 level represents the average of the best existing  performances ot
 plants  within the industry of various  ages,  sizes, processes, or
 other common characteristics.  When existing performance is uni-
 formly inadequate, BPT may be transferred from a.different sub-
 category or category.  BPT focuses on  end-of-process treatment
 rather than process changes or internal  controls,  except when
 these technologies are common industry practice.
                                 43

-------
 The cost and benefit inquiry for BPT is a limited balancing, com-
 mitted to EPA's discretion, which does not require the Agency to
 quantify benefits in monetary terms.  See, e.g., American Iron
 and Steel Institute v. EPA, 526 F.2d 1027 (3rd Cir. 1975).	In
 balancing costs against the benefits of effluent reduction, EPA
 considers the volume and nature of existing discharges, the
 volume and nature of discharges expected after application of
 BPT, the general environmental effects of the pollutants, and the
 cost and economic impacts of the required level of pollution con-
 trol.   The Act does not require or permit consideration of water
 quality problems attributable to particular point sources or
 water  quality improvements in particular bodies of water.  There-
 fore,  EPA has not considered these factors.   See Weyerhaeuser
 Company v.  Costle,  590 F.2d 1011 (B.C.  Cir.  1978)TAppalachian
 Power  Company v. Train, 545 F.2d 1351 (D.C.  Cir. 197b)~

 BAT Effluent Limitations

 The factors considered in defining best available technology
 economically achievable (BAT)  include the age of equipment and
 facilities  involved,  the processes used,  process changes, and
 engineering^aspects  of the technology process changes,  non-water
 quality environmental impacts  (including energy requirements)  and
 the costs of applying such technology [(Section 304(b)(2)(B))].
 At  a mininum,  the BAT level represents  the best economically
 achievable  performance of plants  of various  ages,  sizes,  proces-
 ses, or other shared  characteristics.'  As  with BPT,  uniformly
 inadequate  performance within  a  category  or  subcategory may
 require transfer of  BAT from a different  subcategory or category.
 Unlike  BPT,  however,  BAT may include process  changes  or internal
 controls, even  when  these technologies  are not common industry
 practice.

 The  statutory assessment  of BAT  "considers"  costs, but  does  not
 require a balancing of costs against effluent  reduction benefits
 vsee Weyerhaeuser v.  Costle, supra).  In developing  the proposed
 BAT> however, EPA has  given substantial weight  to  the reasonable-
 ness of costs.   The Agency  has considered  the  volume  and  nature
 of  discharges,  the volume  and nature of discharges expected  after
 application of  BAT, the general environmental  effects of  the
 pollutants, and the costs  and economic  impacts  of  the required
 pollution control levels.   Despite this expanded consideration of
 costs,  the primary factor  for determining  BAT  is the  effluent
 reduction capability of the control  technology.  The  Clean Water
Act^of  1977 establishes the achievement of BAT  as  the principal
national means  of controlling toxic water pollution from  direct
 discharging plants.
                               44

-------
BCT Effluent Limitations

The 1977 Amendments added Section 301(b)(2)(E) to the Act estab-
lishing "best conventional pollutant  control technology   (BCT)
for discharges of conventional pollutants  from existing  indus-
trial point sources.  Conventional pollutants are those  defined
in Section 304(a)(4)  [biological oxygen  demanding pollutants
(BOD), total suspended solids  (TSS),  fecal  coliform, and pHJ, and
any additional pollutants defined by  the Administrator as
"conventional" [oil and grease, 44 FR 44501, July 30, 1979J.

BCT is not an additional limitation but  replaces BAT for the  con-
trol of conventional  pollutants.  In  addition to other factors
specified in Section  304(b)(4)(B), the Act  requires that BCT
limitations be assessed in  light  of a two-part "cost reasonable-
ness" test.  American Paper  Institute v. EPA, 660 F.2d 954  (4th
Cir. 1981).  The  first test  compares  the costs for  private  indus-
try to reduce its conventional pollutants  with the  costs to
publicly owned treatment works for similar levels of reduction  in
their discharge of  these pollutants.   The  second test examines
the cost effectiveness of additional  industrial  treatment beyond
BPT.  EPA must find that limitations  are "reasonable" under both
tests before establishing them as BCT.  In no case  may BCT  be
less stringent than BPT.

EPA published its methodology  for carrying out the  BCT analysis
on August  19, 1979  (44 FR  50732).   In the  case mentioned above,
the Court of Appeals  ordered EPA  to  correct data errors  underly-
ing EPA's  calculation of the first  test  and to apply  the second
cost test.   (EPA  had  argued that  a  second  cost test was  not
required.)

On October  29,  1982,  the Agency proposed a revised  BCT methodol-
•ogy.  We are deferring proposal of  BCT limitations  for  this
category until we can apply the revised  methodology to  the tech-
nologies available  for the  control  of conventional  pollutants in
this  category.

New Source Performance Standards

The basis  for  new source  performance standards  (NSPS)  under
 Section 306 of  the Act  is  the best  available demonstrated tech-
nology  (BDT).   New plants  have the  opportunity to design the best
 and most efficient processes and  wastewater treatment technolo-
 gies.   Therefore, Congress  directed EPA to consider the best
 demonstrated process  changes,  in-plant controls, and end-of-
process treatment technologies that reduce pollution to the
maximum extent  feasible.
                                45

-------
 Pretreatment Standards for Existing Sources

 Section 307(b) of the Act requires EPA to promulgate pretreatment
 standards for existing sources (PSES) which industry must achieve
 within three years of promulgation.  PSES are designed to prevent
 the iatroduction of pollutants into a POTW that pass through,
 interfere with, or are otherwise incompatible with the operation
 of POTW.

 The legislative history of the 1977 Act indicates that pretreat-
 ment standards are to be technology-based, analogous to the best
 available technology for removal of toxic pollutants.  The
 General Pretreatment Regulations which serve as the framework for
 the proposed pretreatment standards are in 40 CFR Part 403 (46 FR
 9404 (January 28,  1981)).

 Before proposing pretreatment standards,  the Agency examines
 whether the  pollutants discharged by the  industry pass through
 the POTW.   In determining whether pollutants pass through a POTW,
 the Agency compares the percentage of a pollutant removed by POTW
 with the  percentage removed by direct dischargers applying the
 best available technology economically achievable.   A pollutant
 is  deemed to pass  through the POTW when the average percentage
 removed nationwide by well-operated POTW  meeting secondary
 treatment requirements, is less than the  percentage removed by
 direct dischargers complying with BAT effluent limitations guide-
 lines  for that pollutant.

 This definition of pass through satisfies two  competing objec-
 tives  set  by  Congress:   (1)  that  standards for indirect dis-
 chargers  be  equivalent to  standards for direct dischargers,
 while,  at  the same time,  (2)  that the  treatment  capability and
 performance  of the POTW be recognized  and taken  into  account in
 regulating the discharge  of  pollutants  from, indirect  dischargers.
 The  Agency compares  percentage removal  rather  than  the mass  or
 concentration of pollutants  discharged  because the  latter would
 not  take  into account  the  mass of pollutants discharged to the
 POTW from  non-industrial  sources  nor the  dilution of  the  pollu-
 tants  in  the  POTW  effluent to  lower concentrations  due to the
 addition of large  amounts  of non-industrial wastewater.

 Pretreatment  Standards  for New Sources

 Section 307(c) of  the Act  requires  EPA  to  promulgate  pretreatment
 standards  for  new  sources  (PSNS)  at the same time that  it promul-
gates NSPS.   These standards are  intended  to prevent  the  dis-
 charge of pollutants which pass through,  interfere  with,  or  are
otherwise incompatible with a  POTW.  New  indirect dischargers,
 like new direct dischargers, have  the opportunity to  incorporate
the best available demonstrated technologies --  including  process
                               46

-------
changes, in-plant controls, and end-of-process treatment technol-
ogies -- and to select plant sites that ensure the treatment
system will be adequately installed.  Therefore, the Agency sets
PSNS after considering the same criteria considered for NSPS.
PSNS will have environmental benefits similar to those from NSPS.

DATA GATHERING

In 1977-1978, under the authority of Section 308 of the Clean
Water Act, data collection portfolios (dcp) were mailed to 475
companies identified in a Dun and Bradstreet list as companies
believed to be active in copper forming.  Responses were received
from approximately 85 percent of the 475 companies originally
contacted.  The responses provided information on 176 plants that
perform manufacturing operations covered under the Copper Forming
Point Source Category.

In addition to the above data sources, EPA visited 12 copper
forming plants.  Plant visits were made to sample wastewater
sources and treatment effluents and to gather additional informa-
tion on manufacturing processes, wastewater  flows, and wastewater
treatment technologies and associated costs.  Samples were col-
lected at these 12 plants in order to characterize the waste-
waters from all of the copper forming manufacturing operations
and to characterize the performance of existing  treatment sys-
tems.  As such, the 12 plants selected for sampling are typically
plants which practice multiple  forming operations and associated
surface and heat treatment operations.  The  12 sampled plants^
typically practice some combination of hot rolling, cold rolling,
drawing, extrusion, and forging, as well as  the  ancillary opera-
tions of solution heat treatment, alkaline cleaning, annealing,
and pickling.  The flow rates and pollutant  concentrations  in  the
wastewaters discharged from the manufacturing operations at  these
plants are representative of the flow rates  and  pollutant concen-
trations which would be found in wastewaters generated by similar
operations at any plant in the  copper forming industry.

The Agency also collected information on treatment systems  not
currently used in the industry.  To collect  this information,  EPA
surveyed literature, contacted  waste treatment equipment manu-
facturers, and observed applicable  treatment systems used  in
o ther indus tr ie s.

Data related to the performance of  the various treatment  tech-
nology  options considered was obtained  from  copper  forming  and
other industries with similar wastewater.  Performance data  for
chemical precipitation and  sedimentation  is  a  composite  of  EPA
sampling and analysis data  from aluminum  forming, battery-
manufacturing, copper forming,  coil  coating,  and porcelain^
enameling.   Data on the performance of  filtration was  obtained
                                47

-------
 from procelain enameling and nonferrous  metals  manufacture.
 Section VII  (p.253)  presents a detailed  discussion  of  the  data
 bases for lime and settle performance  and lime,  settle and
 filtration performance.

 To obtain economic data,  EPA mailed  an economic  survey question-
 naire to  all plants  known or believed  to be  copper  formers.  This
 survey was mailed  under  the  authority  of Section 308 of the Clean
 Water Act.   The Agency received 103  responses  for the  176  copper
 formers.   The survey was  designed  to provide accurate  and  current
 information  on the economic  and financial characteristics  of the
 industry.  Data collected included information  on market struc-
 ture,  profitability, and  investment  in new capital  and production
 costs.  The  Agency also  collected  information  from  plant visits
 and  personal contacts within industry.

 In addition  to the foregoing data  sources, supplementary data
 were obtained from NPDES  permit files  in EPA regional  offices and
 contacts  with state  pollution control  offices.   The concentration
 or mass loading of pollutant parameters  in wastewater  effluent
 discharges are monitored  and reported  as  required by individual
 state agencies.  These historical  data are available from  NPDES
 monitoring reports.

 OVERVIEW  OF  THE INDUSTRY

 The  copper forming category  consists of  plants which roll, draw,
 extrude,  and forge copper and copper alloys.  Based on informa-
 tion from copper plant data  collection portfolios (dcp), there
 are  approximately  176 facilities in  the  copper  forming industry,
 each employing from  two to 1,500 employees.  There  are a total of
 12,000  employees involved in the forming  of  copper  and copper
 alloys.   Total industry production capacity  is  estimated to be
 3.5  x 10y kg per year (7.7 x 109 pounds per  year) with indi-
 vidual  plant production ranging from 22,700  to 227,000,000 kg
 (50,000 to 500,000,000 pounds)  per year.

Most  of the  copper forming facilities  are  located in the north-
 eastern portion of the United States with  the remainder fairly
 evenly  distributed throughout  the  country.

Figure III-l  and Table III-l  (pp.  58 and 59, respectively) show
 the  geographical distribution of copper  forming plants.

Products  and Product Uses                  i

There  are  six  types  of products made in copper forming plants.
They are plate, sheet,  strip, wire,  rod, tube, and  forgings.
Plate  is  a wide rigid piece  of  metal usually over 1/4  inch thick.
Printing plates were often made from copper, as are plate heat
                                48

-------
 exchangers  and some chemical processing vessels.   Sheet is a wide
 piece  of metal having little rigidity and usually less  than 1/4
 inch thick.   With strip,  the length is many times the breadth and
 the product is commonly handled as coils of metal.  Its uses
 include roof gutters, gaskets,  radio parts, trim, weather strip,
 washers, diaphragms,  etc.   Wire is usually circular in  cross
 section and is flexible.   Rod is similar to wire in that it has a
 circular cross section but is more rigid. Rod and wire  are used
 for screening, fasteners,  jewelry, cotter pins,  lock washers,
 springs, truss wire,  wire brushes, welding rods, chains, hooks,
 and electrical conductors.  Wire, twisted or woven into strands,
 used for lifting or in structural supports, is known as cable.
 Tubing is material in the form of long hollow cylinders.  In
 general, it is used for transporting fluids and heat transfer
 applications.  Specifically, it is used for gas lines;  heater
 lines; oil burner tubes;  plumbing pipe and tube; refrigerators;
 condensers; evaporators;  heat-exchanger tubes; dairy tubes, and
 hydraulic lines.

 Approximately two thirds of all formed copper and copper alloy
 products are  in the  form of bar and wire.  Sheet, strip, and
 plate comprise approximately 20 percent of the copper formed.
 Tube and pipe formed for plumbing and commercial  applications
 account for approximately 9 and 8 percent respectively of the
 total copper  formed.  Table III-2 (p. 60 )  summarizes the distri-
 bution of copper forming products over the last two decades.

 Building construction is the largest end user of  formed copper
 materials,  representing approximately 30 percent  of the total
 demand.  Electrical  and electronic products represent approxi-
 mately 28 percent, followed by  industrial  machinery and equipment
 with approximately 18 percent of  the demand,  consumer products
 with 14 percent and  transportation with 10 percent.  Table  III-J
 (p.61  ) summarizes the distribution  of  formed copper product
 usage.

 Raw Materials

 Raw materials for  copper  forming originate in the casting proces-
 ses in  copper refineries.   Common materials  are  wirebars,  cakes
 or slabs,  and billets.  Typical dimensions are:

 -   Wirebar -  approximately 9  to 13  cm (3.5 to 5  inches)  square
     cross  section,  usually from 1 to  1.4 meters  (38  to  54  inches)
" "   in length and weighing from 61 to 190 kg (135 to 420 pounds).
     Used for rod and  wire.

 -   Cake -  rectangular in  cross  section with ranging weights
     from 63 to 1,800  kg (140 to 4,000 pounds)  or more.   Used for
     plate,  sheet,  and strip.
                                 49

-------
 -   Billet  -  circular in cross section,  usually 7.5 to 38 cm
    (3  to 15  inches  in diameter),  and in lengths up to 132 cm
    (52 inches);  weighs from 254 to 3,810 kg (100 to 1,500
    pounds).   Used  for rod and tubing.

 In  some instances  the raw material is  obtained from a copper
 forming process  at  another mill.   These mills obtain rod, wire
 and strip  and further reduce its  gauge  to customer specifications
 by  redrawing or  rerolling.

 Raw materials used  by copper forming plants may not consist of
 pure copper.   In determining end  uses of copper,  the properties
 of  major significance are electrical conductivity, thermal
 conductivity,  corrosion resistance,  machinability, formability,
 and strength.  When it is desirable  to  improve certain of these
 basic  properties, especially strength,  and an improvement is to
 be  gained  without  significantly sacrificing other important
 properties,  alloying (the dissolution of another metal in the
 copper) is often practiced.   Brasses (Cu-Zn alloys), bronze
 (Cu-Sn alloys),  and other alloys  are frequently produced in all
 of  the common forms.   The principal  classes of alloys are listed
 below  by composition:

     Copper-zinc (binary brasses)
     Copper-tin  (binary bronze)
     Copper-zinc-tin (special brasses and bronzes)
     Copper-zinc-lead and copper-tin-lead (leaded brasses and
           bronzes)                 '
     Copper-zinc-nickels (nickel  silvers)
     Copper-zinc-manganese w/wo tin,  iron or aluminum (manganese
           bronzes)
     Copper-tin-phosphorus  (phosphor bronzes)
        Copper  aluminum w/wo  iron  nickel,  or manganese (aluminum
           bronzes)
     Copper-silicon plus manganese,  tin,  iron,  or zinc (silicon
           bronzes)
     Copper-nickel  (cupronickel)
     Copper-beryllium and copper-cobalt-beryllium
           (beryllium-copper)

MANUFACTURING  PROCESSES

Copper  forming manufacturing  facilities  use five  basic techniques
 to  form copper:  hot  rolling,  cold rolling,  extrusion,  drawing,
and  forging.   In addition to  these forming operations,  there are
four surface and heat  treatment processes which impart desired
surface and physical  properties to the  metal.   These ancillary
operations include  annealing,  pickling,  alkaline  cleaning,  and
solution heat  treatment  (commonly referred to  as  quenching).
These  four ancillary  operations result  in nine  distinct  waste-
water  streams  as discussed in Section V.   Casting is not included
in the Copper  Forming  Point  Source Category;  it is regulated
under  the  Metal  Foundaries Point  Source  Category.
                               50

-------
Table III-4 presents information on the number of plants practic-
ing the various manufacturing operations in the copper forming
industry.  It can be seen that drawing is the most commonly
practiced forming operation at copper forming plants.  Of the 88
plants which practice drawing, 70 practice no other forming
operations.  Most plants which practice drawing also practice
annealing.

There are approximately equal numbers of plants which practice
hot rolling, cold rolling, and extrusion (26, 28, and 23 respec-
tively).  Approximately one third of these plants practice only
one forming operation.  The remaining plants practice various
combinations of the five major forming operations.  Most plants
which practice hot rolling, cold rolling or extrusion also
practice solution heat treatment, alkaline cleaning, annealing,
and pickling.  Only six plants in the copper forming industry
practice forging.  Most of these plants also practice pickling of
the forged products.

Each of the forming and ancillary operations is briefly described
in the  following paragraphs with an emphasis on where water  is
used and how pollutants are generated.

Hot Rolling

Rolling  is used to transform  cast copper into one of a number of
intermediate or final products.  Pressure  exerted by the rolls as
copper  is passed between them reduces the  thickness  of the metal.
Hot rolling  is rolling that occurs at an elevated temperature but
most importantly, above the recrystallization temperature of the
metal.   The  recrystallization temperature  is the  temperature at
which the  metal crystal structure becomes  reoriented, and con-
sequently  the  metal becomes more  soft and  ductile.

Lubricants  are used during hot  rolling  to  prevent excessive  wear
on the  rolls.  Since  the metal  is  soft  and ductile  it requires
very  little  lubrication.   Most  plants use  dilute  oil—water
mixtures (<4 percent  oil by volume) or  water alone  as a  lubri-
cant.   The lubricant  also  serves  to  cool  the rolls  during pro-
cessing.   Maintenance of  a uniform temperature  distribution
across  the rolls  is essential to  maintaining a  product with  uni-
form  thickness.   The  use  of  deionized water to  replace^evapora-
tive  and carryover  losses  and the addition of bactericides  and
antioxidizing  agents  are  practiced at many plants  to increase  the
 life  of the lubricants.  Nevertheless,  the lubricant eventually
becomes degraded  and  must  be  eliminated from circulation either
by  continuous  bleed or  periodic discharge.  The discharge  con-
tains  trace organics, toxic  metals,  oil and grease, and  suspended
 solids.  Oil and grease and  toxic organics present  in the dis-
 charge  apparently originate  in the lubricants used.  Suspended
 solids  and toxic metals  present in the discharge result  from
contact of the water  or lubricant solution with the copper
 product or rolls.
                                 51

-------
 Cold Rolling

 Cold rolling uses equipment that is similar to that used in hot
 rolling;  however, it occurs at temperatures below the recrystal-
 lization point of the copper;   The copper is harder and less
 ductile,  requiring more lubrication than in hot rolling.   The
 lubricant also functions as a  cooling medium but to a lesser
 extent  than in hot rolling. The lubricants used in cold rolling
 consist of more concentrated oil--water mixtures to reduce the
 frictional resistance on the surface of the copper and the rolls.
 Spent cold rolling lubricants  are often filtered or allowed to
 settle  in tanks to remove metal fines and other contaminants and
 subsequently recirculated through the rolling mills.   As  is the
 case with hot rolling lubricants,  it is necessary to  periodically
 batch discharge and replace the lubricant.   The pollutants found
 in  the  spent lubricant discharge are toxic  organics,  toxic
 metals,  oil and grease,  and suspended solids.   These  pollutants
 are present as a result  of the use of the oil--water  lubricants
 and the direct contact of the  lubricant with the metal being
 rolled.                                     ;
                                            i
 Extrus ion

 Extrusion is a hot deformation process  which is used  to produce
 tubing, round and shaped (e.g.,  hexagonal,  square)  rod,  and
 extruded  shapes  of many  different  cross sections using billets  as
 the raw material.   In extrusion,  copper is  forced through  an
 orifice (die)  and emerges  in the desired shape.   Extrusion speed
 is  temperature dependent and temperatures may  range - from 650  to
 1,100°C  (1,200°  to 2,000°F).   As  such,  considerable heat is
 generated by the process;  if the extrusion  rate is  high, improp-
 erly dissipated  heat  may result  in temperatures sufficiently high
 to  melt or induce cracking in  the  metal.  Water based lubricants
 are  generally  not used to  control  temperature,  rather,  the
 extruded  copper may be heat treated on  the  press (refer to
 Solution Heat  Treatment  discussion which follows).

 Drawing

Drawing is  a process  in  which  wire  or tubing is  pulled  through  a
 die  to  reduce  the cross-sectional  area.   Wire  is drawn  (pulled)
 cold through a  series  of tungsten  carbide dies,  decreasing the
 diameter  in each draw.   Diamond  dies  are used  for fine wire.
Temperature  rise  is important  because of its relation  to die life
 and  lubrication.  Water-based  lubricants  are used to  control and
to lubricate the  copper  as  it  is drawn  through  the  die.  The
 lubricant  solution eventually  becomes degraded  and  must be
periodically discharged  and replaced.  Pollutants present  in the
discharge  include  toxic  organics,  toxic  metals,  oil and grease,
and suspended  solids.  Toxic organics and oil and grease present
 in the discharge  apparently originate in  the lubricants used.
                                52

-------
Toxic metals and suspended solids appear in the spent lubricants
as a result of the direct contact with the metal and dies during
the drawing process.

Forging

Forging is the forming of metal, usually hot, by individual and
intermittent applications of pressure.  Forging may be done in
open or closed dies.  Products are normally turned out as dis-
crete pieces rather than as a continuous flowing mass.  Forging
requires that the material be heated uniformly to the proper
temperature.  Maintenance of the uniform temperature distribution
throughout the workpiece is easier to control in forging than in
the other forming operations.  Since there is no requirement for
a supplemental cooling medium and the products are turned out as
discrete pieces, lubricants are not required when forging copper.
Consequently, there is no discharge of wastewater from forging of
copper.

Annealing

Annealing involves heating the copper or copper alloy to an ele-
vated temperature (350° to 850°C) during rolling operations to
reduce stresses introduced into the metal.  It is accomplished in
a variety of equipment differing in method of heating, annealing
atmosphere, and mode of of operation.  Plants commonly have
multiple annealing units with several types of equipment
represented.

Most annealing units are heated by the combustion of natural gas
with the heat transferred by direct radiation and convection
from the flame to the product.  In some cases a secondary trans-
fer medium  (commonly partially burned gas) may be employed.  In
annealing wire, some units apply heat by passing electrical
current directly through the wire.  These "electroneal" units
achieve exceptionally high heating efficiency and temperature
control.

In addition  to generating heat, the combustion of natural gas ^ may
be used to generate an "inert" or reducing atmosphere with which
the annealing furnace may be filled to reduce surface oxidation
which would  otherwise occur at the elevated temperatures
employed.  Older furnaces without atmosphere  control yield
annealed products with oxidized surfaces.  The control of surface
oxidation  in annealing not only reduces metal loss  in production,
but also significantly reduces pickling requirements at  later
points  during processing.

Annealing  operations may operate continuously or  on a batch
basis.  Continuous  operation is typified by  electrical anneals,
continuous  roller hearth furnaces,  and  continuous  strip  annealing
                                53

-------
 operations.   In continuous strip and wire annealing operations,
 the product  moves through the furnace as a ! continuous strand,
 while roller hearth furnaces continuously convey discrete coils
 or lengths of product through the furnace.  In either case,  the
 furnace characteristically contains a heating zone, an annealing
 zone at approximately constant temperature, a cooling zone,  and,
 on some units,  a quench.   The quench may consist of a tank
 through which cooling water flows which rapidly dissipates the
 heat at the  surface of the copper or copper alloy.   These water
 quenches are typically discharged continuously to control the
 temperature  in the quench tank.   This discharge contains  toxic
 metals  and suspended solids which result from contact of  the
 quench  water with the heated copper product.

 There are also  package drawing machines which include an  in-line
 annealing furnace followed by a quench, where the quench  medium
 is an oil—water mixture.    These oil--water quenches are typi-
 cally cooled indirectly and are,  therefore, not continuously
 discharged.   The oil—water quench solution must, however, be
 periodically discharged and replaced because of the continuous
 buildup of contaminants.   The spent oil—water quench solution is
 contaminated with toxic organics,  toxic metals,  oil and grease,
 and suspended solids.   Toxic organics and oil and grease  present
 in this discharge apparently originate in the oil used in the
 quench  solution.   Toxic metals  and suspended solids present  in
 the discharge result  from  contact  of the quench solution  with  the
 heated  copper wire.

 Batch annealing  is accomplished  in "bell" anneals which are  gen-
 erally  used  with coiled products.   Coils of products  are  stacked
 and then covered with an air tight jacket.   They are  then heated
 to  the  annealing temperature, maintained there for  a  specified
 period  of time and then cooled by  the use of  non-contact  cooling
 water on the outside  of the  jacket.   After cooling, the jacket is
 removed and  the  annealed coils  are unstacked.   Cycle  times on
 batch annealing  units  are  generally much longer  than  on continu-
 ous  annealing units.   There  is no  contact water used  in batch
 annealing.   Consequently,  there is  no discharge  of  process water
 from batch annealing.

Pickling

Pickling  is  the  use of  acids  (usually sulfuric)  to  remove  surface
oxides which  could interfere with  subsequent  deformation proces-
 ses  or  make  the  finished product less  attractive.   It  generally
occurs  in a bath (tank) and  is followed  by  one or more rinsing
operations to remove  the acid from the  metal  surface,  and often
also involves the use of additional  chemicals  such  as  sodium
dichromate or hydrogen  peroxide to  produce  a  brighter  and more
tarnish resistant finish.
                                54

-------
Except for some bright annealed materials, copper alloys must be:
(1) pickled after each annealing treatment;  (b) completely
descaled (usually); and  (c) in some cases, bright dipped to
produce a color and luster suitable for  final product or further
treatment.  Pickling solutions containing  (by volume) 4 to 15^
percent sulfuric acid are used for the removal of oxides.  Bright
dips consist of sulfuric acid and nitric  acid with  a small amount
of hydrochloric acid, a dichromate dip,  and  a hydrogen peroxide-
acid (usually sulfuric) solution.  Nickel  silvers and cupro-
nickel alloys do not respond readily to  the  pickling solutions
usually used for brasses because nickel  oxide has a limited
solubility in sulfuric acid.  It is desirable to control the
metal surface condition by avoiding oxidation of the metal
especially in the annealing step.  Tubing  made of cupro-nickel
may be annealed in a reducing atmosphere to  produce a clean
surface that does not require acid treatment.  Where pure copper
is pickled with a sulfuric acid solution,  the copper and acid  are
often both recovered using electrolytic  deposition  of copper  from
the spent pickling bath.  Some success has been achieved using
this procedure with alloys and the recent  development of methods
for selectively recovering the various alloy metals shows
promise.

A periodic discharge from the pickling bath  ensures that contami-
nant concentrations will not effect product  quality or  reduce  the
effectiveness of the bath.  The highly acidic nature of the bath
results in high levels of metals  (dissolved) in the bath dis-
charge which originate in the copper product which  is pickled.
Discharges from pickling baths also contain  hexavalent  chromium
which originates in the  dichromate added to  the baths.

Water used for rinsing the pickled copper contains  metals;  how-
ever, they are found at  lower concentrations than  in  the bath.
The higher volume of water used in rinsing acts to  dilute  the
concentrations of the toxic metal  contaminants which  are dragged
out from the pickling bath on the  surface of the  copper product.

Alkaline Cleaning

Alkaline cleaning commonly precedes annealing to  limit  the  amount
of  oil  that  is introduced  into  the  furnace.   It may also follow
annealing  and be used to remove the resulting tarnish and^smut.
Vapor or  solvent  degreasing may be used  in place  of alkaline
cleaning.  There  is no water used  in vapor or solvent  degreasing.

A  typical  alkaline  cleaning operation  consists  of a bath (tank)
in  which  the product  is  dipped  and a  series  of water  rinses to
remove  the entrained process  solutions  (drag out)  and the
contaminants contained  therein.
                                55

-------
A typical alkaline cleaning solution may  contain  from 10 to 20
percent caustic, from 5 to 20 percent sodium polyphosphate, from
30 to 50 percent silicates, from 0 to 25  percent  sodium  (bi)
carbonate, from 5 to 10 percent resin type  soap,  2 to 10 percent
organic emulsifier, as well as wetting agents and chelating
agents.  To properly control the concentration of impurities, a
portion of the bath is continuously or periodically discharged.
The discharge will contain toxic organics,  toxic  metals, oil and
grease, and suspended solids.  The toxic  organics and oil and
grease present in the discharge apparently  originate in the
lubricants which are cleaned from the surface of  the copper prod-
uct toxic metals and suspended solids present in  the discharge
are also washed from the product surface  and originate in the
forming operation which preceeds alkaline cleaning.

Water used for rinsing contains oil and grease as well as metals,
however in a much lower concentration than  in the bath.  The
higher volume of water used in rinsing acts to dilute the
concentrations of these contaminants.

Solution Heat Treatment

In the copper forming industry, solution  heat treatment refers to
the practice of quenching formed copper products  in water or an
oil—water solution in order to reduce thei  temperature of the
workpiece when it leaves the forming operation.   The purpose of
this quenching is to impart desired mechanical properties to the
product and to facilitate handling and further working of the
product.  Solution heat treatment is practiced following all of
the major forming operations; however, it is most commonly used
following hot rolling and extrusion because of the high tempera-
tures at which these operations are performed.  Quenching is
typically achieved by immersing the workpiece in  a tank through
which the cooling water flows.  Spray quenching is also prac-
ticed.  Water is used exclusively as the  quenching medium for
solution heat treatment of copper products  following all of the
major forming operations except extrusion.  In the case of
extrusion, an oil—water solution is sometimes used.

Quench water from solution heat treatment is typically discharged
continuously to control the temperature in  the quench tank.  Pol-
lutants present in the discharge from solution heat treatment
water quenches include toxic organics, toxic metals, oil and
grease, and suspended solids.  Toxic organics and oil and grease
present in the quench water discharge apparently  originate in the
lubricants used in the forming operations which preceed solution
heat treatment.  Toxic metals and suspended solids present in
quench water discharges also originate in the forming operations
which preceed solution heat treatment and also result from
contact of the quench water with the surface of the hot copper
product.
                               56

-------
In the case of extrusion, where oil--water mixtures are^used as
the quenching medium, the quench solution is cooled indirectly
and is  therefore, not continuously discharged.  These oil—water
quench solutions must be periodically dumped and replaced,
because of the continuous buildup of contaminants.  The pollu-
tants and sources of pollutants found in this discharge are the
same as those for continuous discharges from solution heat
treatment water quenches.  Additionally, toxic organics^and orl^
and grease are apparently contributed by the oil which is used in
the oil--water quench solution.
                                 57

-------
                                                                                                           I
                                                                                                           H
                                                                                                           M
                                                                                                           M
                                                                                                          •H
                                                                                                                S3
                                                                                                                O
                                                                                                                H
                                                                                                                to
                                                                                                                £3
                                                                                                                Q
                                                                                                                J25
                                                                                                           S    B
                                                                                                                PM
                                                                                                                PH
                                                                                                                O
                                                                                                                §
                                                                                                                M
                                                                                                                H
                                                                                                                H
                                                                                                                CO
                                                                                                                H
                                                                                                                Q
                                                                   58
_

-------
                          Table III-l

       GEOGRAPHIC DISTRIBUTION OF COPPER FORMING INDUSTRY
              IN THE UNITED STATES BY EPA REGIONS
         Percent of All
*Percent of Upper
50 Percentile of
  Percent of
Copper Forming
Plants Adjusted
EPA
Region
1
2
3
4
5
6
7
8
9
10
Copper Forming
Plants
30.2
13.2
7.8
8.5
22.5
6.2
3.9
0
7.7
0
Copper Forming
Plants
27.8
15.3
9.7
8.3
22.3
6.9
2.8
0
6.9
0
For Regron Pop-
ulation
47.0
12.0
8.3
5.2
10.1
6.8
4.3
0
6.2
0
*Plants having more than 4,000 metric tons (8,740 k pounds)
 annual production.
                               59

-------
 CO
 H
 O
 H)
 Q


 I
CO
                 CO  CO
                 a  c!
                 O  O
                   Q)
                O M-l
                   cd
                •p'.
                c o 
-------












CO
|
H
H
M

CD
rH
rO.
CtJ
H









&
0
H
H
^
PQ
H
£
CO
H
Q
• W
•$
CO
p

H
CJ
C->
Q
O
P4
S
Pi
M
PM
Pn
O
O
Q
O
fe

CO
4-1
CJ
Tl
w
O
M
PM









































o co o
•H CO £3 *rJ
4J 4-> O J-I/-N
W 0) -H 4-) CO
O CD ^ rH CD fi
II C3 li _j »^-i (^
•M w H rH ^  4^
4J -H W C
(3 M CD CD
d) 4-1 £3 rO S
Orrt -^ f* ^
uj »rM V-i M.
!M ^ ^d ^ «H
<1) 'o O 0
p\ j (3 c^ O"
MS w
M CO
JJ CD rH 4J
fl S cd o
i cil '"I ^rl LJ ^
\U r- ' W " ,«!
O 03 C< Q) 'O
yj d cp ri o
CD O CD M
PL, 0 O PL,
1
4J 4J
(3 M
CD 0 (3
OQj d
M-< W
M co «H
CD d 4J
PL, ccf
M
H
I
4J bO O
C fi d
CD -in H C
M rH CQ«rH
CD -H C! 4J
PL, 3 O
M U
J-l
cd
CD
^-i



i — ^coinoOrHco-d'inmo
ONCMvDrHr-^OOOOvOrH
rHCMCMcOCMCOCOCMCMCO





ocMmr-~-ooo<|-ooo
cocMcMco
-------
Multiple Forming
Operation Plants
00 00 00 CM OO
                                O
                                u-i
                                 -rl
                                 0





t
w
H
H

CD
rH
•s
H



























ANUFACTURI;
INDUSTRY
s
CJJ
co !S
8S
H p4
gg
^

rh rTi
JgJ p .
M PM
00
H 0
o*w
*^J p^
o^ ^— i
PM

CO H
HP OT
1-4 O
PM M
PP ^
o p2
w

w o
p^
s
^~l
j2;











Forming
on Plants
CD .rl
rH 4J
60 cd
PS rl
•H CD
co a
0
00 O OrH CO
^^ r*^ i"1 1






rl
CD
_Q CO
§4J
a
i— I PM
cd
4J M-4
0 0
E-*




VO OO CO CO vO
CN] C>1 GO C>4






4J
p<
n\
p!
0
•rl
4J
C$
j-i
rl '
o :
O1^ CO
M ^
0) (1)
4J 4J
cd cd

4-3 4J
.H -rl
^ ^

L^| O
CM m
N«-^ ^-^ r
r^
£3
4J cd
cd a)

-------
                            SECTION IV

                    INDUSTRY SUBCATEGORIZATION
In developing regulations for the copper forming industry, the
Agency considered whether different effluent limitations and
standards are appropriate for different segments of the industry.
The Act allows that EPA consider a number of factors to deter-
mine if subcategorization is needed.  These factors include raw
materials, final products, plant size, plant age, manufacturing
processes, geographical location, and nonwater quality environ-
mental impacts including energy costs and solid waste generation.

The factors which were considered as a basis for subcategoriza-
tion of the copper forming category are discussed below.  After
consideration of all these factors, the Agency has determined
that the Copper Forming Category is most appropriately regulated
as a single category.

Raw Materials

The raw materials used in the copper forming category can be
classified as follows:

        Copper and copper alloys,

        Lubricants, and

        Surface treatment and degreasing chemicals.

While  raw materials affect wastewater characteristics,  the  type
and amounts of pollutants generated by  the  forming of various
copper and copper alloys are not sufficiently  different as  to
require different limitations or treatment.  Plants  processing
brass  (copper-zinc alloy) will  generally have  higher levels of
zinc  in the wastewater than  in  plants processing pure  copper;
however,  the  streams at both plants are ameanable to the^same
type  of treatment, chemical  precipitation  and  sedimentation,  and
upon  application  of this  treatment will achieve  the  same  effluent
concentration of  zinc.  Refer to Section VII  (p.253) for  further
discussion of treatment  system  performance.  In  addition,  the
types  of  raw  materials used  by  a plant  vary frequently  depending
upon  customer demand.  Subcategorization on the  basis  of  differ-
ent  raw materials would  necessitate that a plant meet  different
limitations each  time  its raw material  varied.

Final Products

While the products  manufactured at  a  copper forming  plant affect
the wastewater  characteristics  to  some  extent, it is not  possible
                                63

-------
 to  establish different  effluent  limitations  for any copper form-
 ing segment  based  on  this  parameter.  A particular product can be
 made using various forming and ancillary operations.   Because the
 various  operations result  in  substantially different  flows per
 unit of  production, it  is  not possible  to relate final products
 to  wastewater characteristics in a  manner that  would  result in
 equitable mass limitations for the  copper forming category.   For
 example, sheet can be made using hot  rolling alone or by using
 hot rolling  followed  by cold  rolling, annealing,  and  pickling.
 The particular process  or  processes used will depend  upon  the
 copper alloy used  and the  customer  specifications;  both of which
 vary frequently.

 Plant Size                                 i

 The number of employees and amount  of production can  be used to
 measure  relative sizes  of  copper forming plants.   However,
 neither  factor provided an adequate basis ;for subcategorization.

 Wastewaters  are largely independent of  the number of  plant
 employees.   Variations  in  staff  occur for 'many  reasons, including
 shift differences,  clerical and  administrative  support, mainte-
 nance workers,  efficiency  of  plant  operations,  and market
 fluctuations.   Due to these and  other factors,  the number  of
 employees is constantly fluctuating,  making  it  difficult to
 develop  a correlation between the number of  employees  and
 wastewater generation.

While plant  production  can be used  to approximate the  mass  of
 pollutant generated,  the Agency  has determined  that it should not
 be  used  to establish  different effluent  limitations for any
 copper forming segment  for the following reasons:

     (1)  As  previously discussed under  final products, total
          production  will  not account for the various  forming
          and ancillary opertions used and the  associated
          wastewater  characteristics  and flows.

     (2)  While the amount of production signficantly  affects
          the total mass of pollutants,  it; has  little  effect  on
          the types and range of concentrations  of  pollutants
          found in the  wastewater and therefore  there  is little,
          if any,  difference  between  the treatment  technology
          required at small and  large plants.

Plant Age

The  forming  operations  used by copper forming plants have not
 changed basically  over  the past  80  years,  to  the  extent that
                               64

-------
there are significant variations in the manner in which water is
used and discharged, or the way in which pollutants are gener-
ated.  Consequently, EPA deemed it inappropriate to subcategorize
the category based on plant age.

Geographical Location

Location is not a significant factor on which to base subcate-
gorization of the copper forming category.  Most copper forming
plants are located in urban areas; thus, there is no vast dis-
parity in land availability.   In addition, few plants use land
application or evaporation to treat copper forming wastewaters.
Location is therefore not an appropriate basis for subcategoriza-
tion of the copper forming category.

Manufacturing Processes

The copper forming manufacturing processes consist of five
forming processes and nine surface cleaning and heat treatment
processes which impart desired surface and physical properties to
the formed copper product.  The Agency considered subcategorizing
the copper forming category based on the five forming operations
(hot rolling, cold rolling, extrusion, drawing, and forging).
This method of subcategorizing would be consistent with the fact
that plants generally recognize the above forming operations as
unique plant segments and that a signficant number of plants per-
form a single forming operation.  While the Agency considered
subcategorizing on the basis of forming operation performed, we
decided to regulate the category as a single unified subcategory.
This appears to be appropriate in this case because most plants
except those drawing copper use more than one forming operation.

Non-Water Quality Factors

The non-water quality factors of energy usage, air emissions, and
solid waste generation do not provide a basis for subcategorizing
the copper forming category.  After a review of all available
information, the Agency was unable to identify any plant or type
of plant which have an unusual non-water quality associated
impact.  Similarly, energy requirements, in terms of amounts and
availability did not distinguish any particular segment of the
copper forming category.

The Agency considered all of the above factors and none of them
served to identify discrete segments within the category so dif-
ferent as to warrant different limitations.  Conversely, the
Agency found that different processes generated similar waste
streams, treatable by the same technologies to the same level.
                               65

-------
 Therefore,  subcategorization is unnecessary and the category is
 being considered as a single (unified)  subcategory.

 Production  Normalizing Parameter

 In order to ensure equitable regulation of the category,  effluent
 limitations guidelines and standards  of performance have  been
 established on a pollutant mass discharge basis (i.e.,  mass  of
 pollutant discharged per unit of production).   The unit of pro-
 duction specified in these regulations  is known as a production
 normalizing parameter (PNP).   Establishing concentration  limita-
 tions rather than mass-based limits was considered;  however,  a
 plant that  diluted its wastewater would have an advantage in
 meeting concentration-based  limitations over a plant that con-
 served water.   Thus,  with concentration limitations  a plant  might
 actually be penalized for having good water conservation  prac-
 tices.   To  avoid this possibility,  the  mass of pollutants in the
 discharge has_been related to a specific PNP to establish a  limi-
 tation that will limit the pollutant  mass discharged proportion-
 ate to  an amount of production.

 The^approach used in  selecting the appropriate PNP is two-fold:
 achieving a correlation between production and the corresponding
 discharge of pollutants  and  ensuring  feasibility and ease of
 regulation.  Some of  the alternatives considered in  specifying
 the PNP  include:

      1.   Mass  of copper  produced,
      2.   Number of finished  products  manufactured,
      3.   Surface area of copper  processed,  and
      4.   Mass  of process chemicals used.

 The evaluation of these  alternatives  is summarized in the dis-
 cussion  that follows.

 Mass  of  Copper Processed.  The copper forming  industry  typically
 maintains production  records  of  the pounds  of  copper processed by
 an  individual  unit  operation.  Availability  of these production
 data  and lack  of data for other  production  parameters,  such as
 area  of  copper and  number  of  products,  makes this  the most con-
 venient ^ parameter to  use.  The copper forming  dcp  reqttested three
 production values:  the  capacity production  rate for the unit
 operation in question, the maximum production  rate achieved in
 1977, and the  average production rate for 1977,  all  in  Ib/hr.
The^PNP  is based on the  average  production  rates reported in the
dcp's.   In most  cases, the plants were  operating their units at
 or  near  the capacity  production  rate.   The  average production
rate will correlate with the  mass of  pollutants  found in the
wastewater.
                               66

-------
Number of End Products Processed.  The number of products proces-
sed by a given plant would not account for the variations in size
and shape typical of formed products.  Extrusions, for instance,
are produced in a wide range of sizes.  It would be unreasonable
to expect the quenching of a large extrusion to use the same
amount of water required for a smaller extruded product.

Surface Area of Copper Processed.  The area of copper processed
is not generally kept or known by industry.  In some cases, such
as forging of miscellaneous shapes, surface area data would be
difficult to determine.  Surface area data would be difficult to
collect.  Surface area is an appropriate production normalizing
parameter for copper which has been cleaned or etched  (for these
operations, the water use and discharge ought to show a correla-
tion with surface area).

Mass of Process Chemicals Used.  The mass of process chemicals
used (e.g., lubricants, solvents, and cleaning or etching solu-
tions) is dependent on the processes which  the copper undergoes
rather than the copper or copper alloy used in the process.

Selection of the Production Normalizing Parameter

Two of the  four parameters considered, number of  finished prod-
ucts and mass  of process  chemicals  are inappropriate PNP s  for^
the copper  forming category.  The number  of finished products is
inappropriate  because  of  the  lack of  consistency  and uniformity
in the finished products  manufactured by  a  copper-forming plant,
particularly by an extrusion  or  forging plant.  Also  the pro-
cesses vary' from plant to plant  even  when producing essentially
the  same product.  The mass  of process  chemicals  is  an inappro-
priate PNP  because the mass  of pollutants discharged  is more
directly  related  to  the  type  of  operation than  the  amount  of
these process  chemicals used,  even  though the process  chemicals
 frequently  enter  the wastewater.

The  surface area  of  product  as  a PNP  would relate the mass  of
pollutants  discharged to  the  surface area of  copper_that  contacts
 the  process water.   This  parameter would be appropriate for a
 number  of  copper  forming  operations that produce wastewater,
 since  the mass of pollutants entering the wastewater is propor-
 tional  to  the surface area of copper processed.   While this
 parameter may be  appropriate as  a PNP,  copper formed products,
 especially forged products  or extrusions, also  come in a wide
 variety of shapes and the surface area of these shapes would be
 difficult to determine.

 The fourth parameter considered is the mass of product.  The
 Agency has selected mass as the PNP.  The mass of pollutants can
 be related to the mass of copper processed and most companies
                                67

-------
keep production records  in terms  of mass.   The mass  of pollutants
generated  from  each  forming and ancillary  operation  is dependent
on the^mass  of  copper processed through  that  operation.   Thus
there is only one PNP for  each waste stream based  on the  mass'of
copper processed through the operation.

The PNP for  copper forming is "off-kilograms"  or the kilograms  of
product removed  at the end of a forming  or  ancillary process
3K 2^1  ?r £xamPle> in,,the rollin§ Process copper wirebar enters
the mill to be processed.   Following one process cycle which
reduces the wirebarfs thickness and which may  include  multiple
nail passes, the copper  is  removed  from  the rolling  mill.  It may
then be processed through  another operation, such  as  annealing
sizing,  cleaning  or it  may be stored before being brought back
+£  ?v- r1ollinS m:Ll1 for  another process  cycle,  further reducing
the thickness.   The mass of copper  removed  from the rolling mill
after each process cycle multiplied  by the  number  of process
cycles  is the PNP for that process.
                              68

-------
                            SECTION V

             WATER USE AND WASTEWATER CHARACTERISTICS


A description of the sampling and analytical program is presented
below, followed by a description of the process wastewater
sources in the Copper Forming Point Source Category.  The source
of wastewater is discussed in the context of the process which
produces the water.  The amount of water used and wastewater
generated on a production basis is then presented for each of the
fources.  Finally, data from the sampling and analytical program
is presented in tabular form.

SAMPLING AND ANALYTICAL PROGRAM

EPA sampled 12 copper forming plants.  Prior to each sampling
visit  all available data, such as layout and diagrams  of the
selected plant's production processes and wastewater treatment
facilities, were reviewed.  Often a visit to the plant  to be
sampled was made prior to the actual  sampling visit to  finalize
the sampling approach.  Representative sample points were then
selected to provide coverage of discrete raw wastewater sources,
total  raw wastewater entering a wastewater  treatment system,  and
final  effluents.   Finally, before conducting a  visit,  a detailed
sampling plan showing the selected sample points and all perti-
nent  sample data to be obtained was  generated and  reviewed.

The wastewater  sampling program  conducted  at each  plant usually
consisted of screening and verification.   Samples  were collected
over  a three day period.  At  3 plants screening and verification
was undertaken.  Verification  alone  was  performed  at  the remain-
ing plants.  Screening analysis  was  performed  on the  first  day s
samples while verification was performed on samples from days two
and three.  The  objective  of screening was  to  determine which
pollutants were  present  in  the plant wastewater and to quantify
the  levels  of pollutants  present.   Particular  emphasis was  placed
upon  collection  and  analysis  of  samples  for the 129 toxic  pollu-
tants.  Once  the screening data  were obtained,  parameters  were
chosen for  verification  analysis  based on three considerations:
 (1) whether  or  not the  pollutant was detected  during screening;
 (2)  information reported  on the  dcp  concerning the presence or
absence of  the  129 toxic  pollutants; and (3)  technical judgment
concerning  the  probable  presence or  absence of each pollutant.
 Samples collected for verification analysis were preserved
 on-site,  shipped within 24 hours to  the analytical laboratory,
 and extracted.   The extracts were then held until the  screen
 samples were  analyzed.   A more detailed discussion of  sample
 preservation and analysis is presented below.
                                69

-------
 Site Selection

 Twelve copper forming plants were visited for an on-site study of
 their manufacturing processes, water use, and wastewater treat-
 ment.  In addition, wastewater samples were collected at the 12
 plants visited in order to quantify the level of pollutants in
 the waste streams.  The reason that the Agency selected these 12
 plants was to adequately represent the full range of manufactur-
 ing operations found in this industry as well as the performance
 of existing wastewater treatment systems.  As such, the plants
 selected for sampling were typically plants with multiple forming
 operations and associated surface and heat treatment operations.
 The flow rates and pollutant concentrations in the wastewaters
 discharged from the manufacturing operations at these plants are
 representative of the flow rates and pollutant concentrations
 which would be found in wastewaters generated by similar opera-
 tions at any plant in the copper forming industry.  Also,  the 12
 plants selected for sampling have a variety of treatment systems
 in place.   Included in the 12 plants were plants with no treat-
 ment  as  well as plants using the technologies considered as the
 basis for  regulation.

 Pollutants Analyzed

 The chemical pollutants sought in analytical procedures  fall into
 three groups:   Conventional,  nonconventional,  and toxics.   The
 latter group comprises the 129 pollutants found in the priority
 pollutant  list shown in Table V-l.

 Conventional pollutants are  those generally  considered treatable
 by  secondary municipal wastewater treatment.   The conventional
 pollutants  examined for this  study  are:
     .Oil and Grease  (O&G) , and
     'Total Suspended Solids  (TSS).

Nonconventional pollutants are those which  are neither  conven-
tional nor ^ on the list of toxic pollutants.,  The  following
nonconventional pollutants were examined  in the Copper  Forming
Category.  Fluoride, manganese, iron and  phosphorus were  analyzed
because it was anticipated that they might  be present as  a  result
of the alloys processed.  Total organic carbon and total  phenol -
ics were analyzed because they were viewed  as possible  indicators
of the presence or absence of toxic organic pollutants .

     Fluoride,
     Total Organic Carbon,                  '
     Total Phenolics (4AAP) ,
     Manganese,
     Iron, and
     Phosphorus .
                               70

-------
Sampling Methodology

During the initial visit to a facility, a selection was made of
sampling points so as to best characterize process wastes and_
evaluate the efficiency of wastewater treatment.  Representative
sample points were then selected to provide coverage of discrete
raw wastewater sources, total raw wastewater entering a waste-
water treatment system, and final effluents.  The nature of_the
wastewater flow at each selected sampling point then determined
the method of sampling, i.e., automatic composite, grab compos-
ite  or one-time grab sample.  The sample points were individual
raw'waste streams, combined influent to treatment, or treated
effluent.

Each sample was collected by an automatic time  series compositor
over a 24-hour sampling period whenever possible.  When automatic
compositing was not  possible, grab samples were taken at  tnter'
vals over the same period, and were composited  manually.  When a
sample was taken  for analysis of toxic organics,  a blank  was  also
taken to determine the level of contamination inherent to the
sampling and  transportation procedures.

Each sample was divided  into several  fractions  and preserved,
when necessary, in accordance with established  procedures for the
measurement  of  toxic and classical pollutants.  Samples were
shipped in ice-cooled  containers by the best  available route  to
EPA-contracted  laboratories  for  analysis.

Analytical Methods

The analytical  techniques for  the  identification  and quantitation
of toxic pollutants  were those  described  in Sampling and  Analysis
Procedures  for  Screening of Industrial Effluents  for Priority
Pollutants,  revised  in April  1977.

In the  laboratory,  samples for  organic pollutant  analysis were
 separated  by specific  extraction procedures into acid (A),  base-
 neutral (B-N),  and pesticide (P)  fractions.  Volatile organic
 samples (V)  were taken separately as a series of grab samples at
 4-hour intervals  and composited in the laboratory.   The analysis
 of these fractions  included the application of strict quality
 control techniques  including the use of standards,  blanks,  and
 spikes.  Gas chromatography and gas chromatography-mass spec-
 trometry were the analytical procedures used for the organic
 pollutants.   Two other analytical methods were used for the
 measurement of toxic metals:   flameless atomic absorption
 inductively coupled argon plasma spectrometric analysis
 The metals determined by each method were:
                                 71

-------
          Flameless AA
      Antimony
      Arsenic
      Selenium
Silver
Thallium
       ICAP

Cadmium     Lead
Chromium    Nickel
Copper      Zinc
 For the analysis of conventional and nonconventional pollutants
 procedures described by EPA were followed.  The following  con-
 ventions were used in quantifying the levels determined by
 analysis:                                                J

      -  Pollutants detected at levels below the quantification
         limit are reported as "less than"  (<) the quantification
         limit.  All other pollutants are reported as the measured
         value.

      -  Sample Blanks - Blank samples of organic-free distilled
         water were placed adjacent to sampling points to detect
         airborne contamination of water samples.

 WASTEWATER SOURCES

 This  section presents a discussion of the sources of wastewater
 associated with the major manufacturing operations in the copper
 forming industry.   The major sources of wastewater in the copper
 forming industry are lubrication and cooling,  alkaline cleaning
 annealing,  heat treatment, and pickling.   |

 Water  is used for  lubrication and cooling in all of the major
 forming operations  in the copper forming industry.   Two types of
 waste  streams result from lubrication and cooling:   spent lubri-
 cants  and  solution  heat  treatment wastewater.   Spent lubricants
 result from water,  emulsified oils,  or  soluble  oils  that are
 applied directly to the  product  or  the  forming  machine  during the
 forming operation.   The  three specific  spent  lubricant  waste
 streams generated in  the copper  forming  industry  are hot rolling
 spent  lubricants, cold rolling spent lubricants,  and drawing
 spent  lubricants.                                           6

 Process  water is used  in alkaline cleaning  to remove soil and
 lubricants  from the product.   Alkaline cleaning  is usually
 practiced before annealing to  prevent the formation  of  undesira-
ble films on  the metal.  Removal  of  the  soils and  films  after
 annealing is  also sometimes practiced.   Impurities introduced
result  from  cleaning agents and  lubricants, and from residues
 cleaned  from  the metal.  Cleaning  operations may be either
continuous  (typically for  strip)  or  batch operations  (for rod or
tube).   Cleaning is followed by one  or more rinses which produce
most of  the discharge associated with this process.
                               72

-------
Process water use in annealing is primarily for the purpose of
rapidly cooling annealed products in order to limit surface
oxidation and facilitate subsequent handling.  Quenches may be
either aqueous baths in which the product is submerged or sprays
through which the product passes.  The quench solution may
contain only water, or may consist of a soluble oil solution in
water.  Spray quenches generally use water only, while quench
baths are likely to contain soluble oils.  Bell annealing units
do not involve a quench and are most often employed without the
use of process contact wastewater.

Pickling is a. process that removes surface contaminants by solu-
tion  in°an aqueous medium.  Water is used in pickling baths for
the dilution of acids, in rinses used to remove dragout from
pickling baths adhering to product surface, and in some cases, in
wet scrubbers used to control air pollution resulting from
pickling bath fumes.  Wastewater discharges characteristically
result from all three of these process water uses in pickling.

The specific wastewater sources associated with the copper
forming industry are  listed below:

   --Spent Hot Rolling Lubricants,

   --Spent Cold Rolling Lubricants,

   --Spent Drawing Lubricants,

   --Solution Heat Treatment,

   --Extrusion Press  Solution Heat Treatment,

   --Alkaline Cleaning Bath,

   --Alkaline Cleaning Rinse,

   --Annealing Water,

   --Annealing Oil,

    --Pickling Bath,

    --Pickling Rinse,  and

    --Pickling Fume Scrubber.

 A brief discussion of each stream follows:
                                73

-------
Hot Rolling Spent Lubricant

Process water use in hot rolling serves as both a coolant  and  a
lubricant.  Cooling is required in order to  facilitate subsequent
processing; whereas lubrication is needed to reduce  frictional
forces in the metal deformation process.  Cooling is accomplished
by means of on line water sprays during the  actual hot rolling
process.  Lubricants are applied to the rolls either as  soluble
oils or as emulsified oils.

Cold Rolling Spent Lubricant

In cold rolling processes, water is either used in conjunction
with lubricants or as cooling water on the process material or
cold rolling unit.  A variety of lubrication techniques  are used
in processing the metal on the various types of cold rolling
machines.  Emulsified water soluble oils, insoluble  oil/water
mixtures, and mineral oil alone are the main types of lubricants
used.  Cold rolling applied to a previously unrolled slab  direct
from casting (breakdown cold rolling), can be accomplished with-
out lubrication of the process material.  Soluble oil emulsions
and oil lubricants are generally recycled and dumped periodi-
cally.  Insoluble oil lubricants which mix with water and
contaminated cooling water are generally continuously discharged
after contact with the product or mill.  In  most cases,  lubri-
cants are spray applied to the metal*just before it  enters the
rollers, although lubricant is occasionally  swabbed  onto the
metal.  In cases where insoluble oil and water are both  applied
to the metal, they are usually sprayed on simultaneously.

Drawing Spent Lubricants

Process water used in drawing is to provide  cooling  at the die
and as a vehicle for lubrication.  The effects of lubrication  are
to prolong die life, provide a better surface finish on  the drawn
material, remove residues, and increase drawing speed.   In draw-
ing, the lubricant may be sprayed onto the, rod or wire as  it
enters the die or the die may be immersed in lubricant.  Lubri-
cant is commonly recirculated through a lubrication  cooling
system from a holding tank.  Typically, the  contents of  the tank
are contract hauled.

Solution Heat Treatment

Solution heat treatment wastewaters result from cooling  of the
formed copper product after it leaves the forming machine.  Water
is used for quenching copper products from hot rolling,  cold rol-
ling, extrusion, and drawing.  The data indicate that the  flow
rates and raw waste characteristics of solution heat treatment
wastewater are similar regardless of the forming operation which
preceeds the water quench.  Solution heat treatment wastewater
                                74

-------
from water quenching of formed copper products is therefore
considered to be a single waste stream.

Extrusion Press Solution Heat Treatment

Some extrusion quenches, particularly those used for submerged
extrusion, contain emulsified or soluble oils. These quenches are
characteristically recycled and reused.  As a result their dis-
charges are considerably less than those using water quenches.
The waste stream which results from quenching of extruded.copper
products in emulsified or soluble oils is known as  extrusion
press solution heat treatment wastewater.

Alkaline Cleaning Bath

Alkaline cleaning bath wastewaters result from the  periodic dump-
ing of batch  alkaline cleaning baths,  or  a bleed  stream from  a
continuous recirculating alkaline cleaning operation.

Alkaline Cleaning Rinse

Alkaline cleaning rinse wastewaters result  from  the rinsing of
copper produces after alkaline cleaning.  .The  rinsing  operation
may be either spray rinsing or stagnant  rinsing.   The  rinsewater
is  typically  discharged  to  treatment.

Annealing Water

Wastewater  discharge  from spray  quenches results either as water
runs  directly out  of  the  quench  chamber  or  as  a blowdown or
overflow from a quench  water recirculation  system.   Annealing
quench water  is  often mixed with non-contact cooling water and
other process water  in  recirculation systems.   Discharge from
quench baths  may  occur  as  a continuous overflow or as  a periodic
dump  of  the bath.

 Strip is often processed in continuous lines which combine alka-
 line  cleaning, annealing,  and pickling.   The annealing units in
 these lines commonly incorporate a water tank through which the
 strip passes after annealing.  Other products, including coiled
 strip,  are generally quenched by water sprays included as an
 integral part of roller hearth annealing units.

 Annealing Oil

    manv facilities  wire is quenched in baths containing soluble
 os Slfowing continuous annealing.  Annealing oil is associated
 only with drawing operations.  This waste stream is typically
 contract hauled.
                                 75

-------
 Pickling Baths

 Pickling baths are used to remove oxidized metal and other unde-
 sirable contaminants from the surface of copper and copper alloy
 products at various points during and after forming operations.
 In this use the acid content of the bath (generally H2S04)
 becomes depleted and the bath becomes enriched in metals and
 other impurities.   While acid depletion may be overcome by the
 addition of makeup acid, the accumulation of impurities in the
 bath ultimately renders it unfit for continued use.   At that
 point the bath is  commonly discharged and replaced with a fresh
 acid solution.   The pickling bath thus constitutes an intermit-
 tent, low volume,  but very concentrated source of process
 wastewater.

 Pickling Rinse

 Rinses remove dragout from the pickling bath adhering to cleaned
 product surfaces and thus  become contaminated with the materials
 present^in the  bath.   The  wastewater which  results from pickling
 rinses is higher in volume and lower in concentration than
 pickling bath discharges.   The rinse water  is  typically dis-
 charged to treatment.

 Pickling Fume Scrubber

 Wet  scrubbers are  used to  control air emissions which result  from
 the  volatile  components  of pickling  baths and  produce relatively
 dilute waste  streams  similar to those from  pickling  rinses.   The
 fume scrubber wastewater is  discharged to treatment.

 PRODUCTION NORMALIZED  FLOWS

 Wastewater flow rates  are  related  to the amount of production at
 a  given plant.  In order to  take  production into  account,  waste-
 water flow rates are  discussed  in  terms of  production normalized
 flows.   The production normalized  flow is defined  as  the  flow
 rate  of a  given waste  stream  divided by the:production  of  the
 manufacturing operation  associated with the waste  stream.  The
 unit  of production  specified  is known  as the production normal-
 izing parameter (see p.66  ).  Production normalized  flows  are
 expressed  in units  of  liters  of wastewater  per  thousand kilograms
 of product  (1/kkg).

The production  normalized  flows as reported in  the dcp are
presented in Tables V-2  through V-13  for the 12 copper forming
wastewater  streams.  In  addition, these tables  present informa-
tion on reported production and recycle rates.
                               76

-------
POLLUTANTS FOUND AND SOURCES OF THESE POLLUTANTS

Tables V-14 through V-25 summarize the analytical data from each
of the copper forming plants sampled and identifies the specific
waste streams represented by each sample.

The pollutants  found in significant concentrations in copper
forming wastewaters are presented in this section along with a
discussion of the sources of these pollutants  in copper forming
operations.

Toxic Metals

The toxic metals found in significant concentrations in copper-
forming wastewaters are chromium, copper, lead, nickel, and zinc.
                                          f
All of the toxic metals found  in  copper  forming wastewaters in
significant concentrations  (chromium, copper,  lead, nickel, and
zinc) are  found in  copper or copper alloy products either as
alloying additives  or contaminants.  Table  V-26 presents  informa-
tion  supplied, in the dcp from  nine plants on the amounts  of these
metals used as  raw  materials.

Chromium is also added to pickling baths in the form of bichro-
mate  which acts as  a reducing  agent and  imparts desired surface
properties to copper products.  This  is  the source of hexavalent
chromium in pickling bath and  pickling  rinse wastewaters.

Toxic Organics

The  toxic  organic pollutants  found  in significant  concentrations
in copper  forming wastewaters  are benzene,  1,1,1-trichloroethane,;
chloroform, 2,6-dinitrotoluene,  ethylbenzene, methylene  chloride,
naphthalene, N-nitrosodiphenylamine,  anthracene, phenanthrene,
toluene, and  trichloroethylene.

Organic  priority  pollutants found in  copper forming wastewaters
originate  primarily in  the  lubricants used  in the  forming pro-
 cesses.  Published  information on lubricants used  in copper and
 copper  alloy  products  maufacturing  indicate that most  of  the  12
 toxic organic pollutants  found in copper forming wastewaters
 could be present  in these  products.   Most  of these toxic  organ-
 ics,  howeverj  are present  in small  quantities either as  additives
 or as trace  contaminants.   For example,  nonaromatic  chlorinated
 hydrocarbons  are used in stabilized chlorinated oils  which are
used for lubrication under severe conditions.  Specific  compounds
 in this  class such as 1,1,1-trichloroethane and trichloroethylene
 are  commonly used as solvents for oils and fats,  as  are benzene
 and toluene.
                                77

-------
Conventional Pollutants

The  conventional pollutants  found  in  significant  concentrations
in copper forming wastewaters are  oil and grease, and total
suspended solids (TSS).

Oil  and grease found in raw  waste  streams at  copper  forming
plants is primarily attributed to  the lubricants used in the
forming processes.  The lubricants enter wastewater  streams as a
result of deliberate mixing  in soluble or emulsified oil systems,
mixing of fluid lubricants with cooling water on  rolling mills,
solution or entrainment of greases used on roll necks or other
machinery parts in cooling water,  contamination of quench baths
with lubricants from product surfaces, and removal of lubricants
from product surfaces in alkaline  cleaning.

TSS results from the abrasion of particles from the  surface of
the copper product or the surface  of the rolls or dies used in
the major forming operations.  Miscellaneous dirt and particles
as well as soot from annealing furnaces and oxides which form on
the product surface end up in annealing quenches, alkaline clean-
ing, and pickling wastewaters.  Also, suspended solids can form
as a result of chemical precipitation of dissolved solids as
streams of different pH are mixed  deliberately or through dragout
on the product surface.
                               78

-------
                            Table V-l

                   LIST OF 129 TOXIC POLLUTANTS
Compound Name

   1.  acenaphthene
   2.  acrolein
   3.  acrylonitrile
   4.  benzene
   5.  benzidene
   6.  carbon tetrachloride  (tetrachloromethane)

     Chlorinated benzenes  (other than dichlorobenzenes)

   7.  chlorobenzene
   8.  1,2,4-trichlorobenzene
   9.  hexachlorobenzene

     Chlorinated ethanes  (including  1,2-dichloroethane.
     1,1,1-trichloroethane and hexachloroethane)

   10.  1.2-dichloroethane
   11.  1,1,1-trichlorethane
   12.  hexachlorethane
   13.  1,1-dichloroethane
   14.  1,1,2-trichloroethane
   15.  1,1,2,2-tetrachloroethane
   16.  chloroethane

     Chloroalkyl ethers (chloromethyl,  chloroethyl and
     mixed ethers)

   17.  bis (chloromethyl) ether
   18.  bis (2-chloroethyl) ether
   19.   2-chloroethyl vinyl ether  (mixed)

     Chlorinated naphthalene

   20.   2-chloronaphthalene

     Chlorinated  phenols  (other  than those listed elsewhere;
     includes trichlorophenols and chlorinated cresols)

   21.   2,4,6-trichlorophenol
   22.   parachlorometa cresol
   23.   chloroform (trichloromethane)
   24.   2-chlorophenol
                                 79

-------
                       Table V-l (Continued)

                    LIST OF 129 TOXIC POLLUTANTS
   Dichlorobenzenes

25.   1,2-dichlorobenzene
26.   1,3-dichlorobenzene
27.   1,4-dichlorobenzene

   Dlchlorobenzldine

28.   3,3'-dichlorobenzidine

   Dichloroethylenes  (1,1-dichloroethylene  and
   1,2-dichloroethylene)

29.   1,1-dichloroethylene
30.   1,2-trans-dichloroethylene
31.   2,4-dichlorophenol

   Dichloropropane and dlchloropropene

32.   1,2-dichloropropane
33.   1,2-dichloropropylene (1,3-dichlpropropene)
34.   2,4-dimethylphenol

   Dinitrotoluene

35.   2,4-dinitrotoluene                     |
36.   2,6-dinitrotoluene
37.   1,2-diphenylhydrazine                  ;
38.  ethylbenzene
39.   fluoranthene                           ;

   Haloethers (other than those listed elsewhere)

40.   4-chlorophenyl phenyl ether
41.  4-bromophenyl phenyl ether
42.  bis(2-chloroisopropyl) ether
43.  bis(2-choroethoxy) methane

   Halomethanes (other than those listed elsewhere)

44.  methylene chloride  (dichloromethane)
45.  methyl chloride (chloromethane)
46.  methyl bromide (bromomethane)
47.  bromoform (tribromomethane)
48.  dichlorobromomethane
                               80

-------
                      Table V-l (Continued)

                   LIST OF 129 TOXIC POLLUTANTS
49.  trichlorofluoromethane
50.  dichlorodifluoromethane
51.  chlorodibromomethane
52.  hexachlorobutadiene
53.  hexachlorocyclopentadiene
54.  isophorone
55.  naphthalene
56.  nitrobenzene

   Nitrophenols (including 2,4-dinitrophenol and dinitrocresol)

57.  2-nitrophenol
58.  4-nitrophenol
59.  2,4-dinitrophenol
60.  4,6-dinitro-o-cresol

   Nitrosamines

61.  N-nitrosodimethylamine
62.  N-nitrosodiphenylamine
63.  N-nitrosodi-n-propylamine
64.  pentachlorophenol
65.  phenol

   Phthalate esters

66.  bis(2-ethylhexyl) phthalate
67.  butyl benzyl phthalate
68.  di-n-butyl phthalate
69.  di-n-octyl phthalate
70.  diethy1 phthalate
71.  dimethyl  phthalate

   Polynuclear aromatic  hydrocarbons

72.  benzo  (a)anthracene (1,2-benzanthracene)
73.  benzo  (a)pyrene (3,4-benzopyrene)
74.  3,4-benzofluoranthene
75.  benzo(k)fluoranthane  (11,12-benzofluoranthene)
76.  chrysene
77.  acenaphthylene
78.  anthracene
79.  benzo(ghi)perylene  (1,11-benzoperylene)
80.  fluorene
81.  phenanthrene
                                81

-------
                       Table V-l (Continued)

                   LIST OF  129 TOXIC POLLUTANTS


  82.   dibenzo (a,h)anthracene (1,2,5,6-diberizanthracene)
  83.   indeno (1,2,3-cd)pyrene (w,e,-o-phenylenepyrene)
  84.   pyrene
  85.   tetrachloroethylene
  86.   toluene
  87.   trichloroethylene
  88.   vinyl  chloride (chloroethylene)

    Pesticides  and  metabolites

  89.   aldrin
  90.   dieldrin
  91.   chlordane (technical  mixture  and metabolites)
    DDT and  metabolites

  92.  4,4'-DDT
  93.  4,4'-DDE(p,p'DDX)
  94.  4,4'-DDD(p,p'TDE)

    Endosulfan and metabolites

  95.  a-endosulfan-Alpha
  96.  b-endosulfan-Beta
  97.  endosulfan sulfate

    Endrin and metabolites

  98.  endrin
  99.  endrin aldehyde

    Heptachlor and metabolites

100.  heptachlor
101.  heptachlor epoxide

    Hexachlorocyclohexane (all isomers)

102.  a-BHC-Alpha
103.  b-BHC-Beta
104.  r-BHC (lindane)-Gamma
105.  g-BHC-Delta
                               82

-------
                      Table V-l (Continued)

                  LIST OF  129 TOXIC POLLUTANTS
     Polychlorinated biphenyls (PCB's)

106.   PCB-1242 (Arochlor 1242)
107.   PCB-1254 (Arochlor 1254)
108.   PCB-1221 (Arochlor 1221)
109.   PCB-1232 (Arochlor 1232)
110.   PCB-1248 (Arochlor 1248)
111.   PCB-1260 (Arochlor 1260)
112.   PCB-1016 (Arochlor 1016)

     Metals and Cyanide, and Asbestos

114.   antimony
115.   arsenic
116.   asbestos (Fibrous)
117.   beryllium
118.   cadmium
119.   chromium (Total)
120.   copper
121.   cyanide (Total)
122.   lead
123.   mercury
124.   nickel
125.   selenium
126.   silver
127.   thallium
128.   zinc

     Other

113.   toxaphene
129.   2,3,7,8-tetra chlorodibenzo-p-dioxin  (TCDD)
                                83

-------
                  tot)
                  M
                  05
      w
   ,
    O 0)
    W 4J
   •H CO
           t^MMNMHMHHMHHHHQHHHQHHHQQQHQQl-l
            c
            2  b
           •H  >~
           •U-~~
   o m
   MM-l
   pn O
           O ONO
           O CM O
           0
rH



H
O
H

PQ


H?

O

M
                 0) O

                 M a
                 0) 0)
   a)
      W)
              15 .H
                 Q
                             \a\
                                           3 OO
, r~-1— m
  *  •  •
i ON ON r**-' '
i (J^ ON ON
           OOOOOOOO.
-------
                   r-l O OO O CO "1 O. r-H r-| i-H
                                                                              vO
                                                                                 CO M CN CM O
OO
 I
•3
                  4J il)
                  Cr^
                  
-------
                   0)
                   60
                   J-(  CO
                  o oj
                  CO 4J
                  T( CO
                  Q
                           NIN1N1N1N1N1N1N1NINININIMN1NININ1N1NININ1NIN1NININ1NINININI
                  O J-l
                  •H p*


                  3rH

                  o m
                              3OOOOCM|-~OvOOOOOOOOOrHrHtoOOOO
            OOir)CNCMOOOOOtOCOOcOtOOtOCOlOO<±COOOrHOCMONOOCMO
                                   
-------
Discharge
Status
                         NININININININININI
                                                           N1N1N1N1NIN1N1NININ3N1N1NININ1N1NIN1N1
                  d/->
                  O M
                 •rl >,
                  4-»~
   O O CO CO i—I OO in
                         CM   0)

 Q) 'o
 O  ^
 M  O
 0)  0)
PH {£
          O">
                      ON
ION
I ON
         ON

! ON ON OO ON
; ON ON ON ON
| in ON ON ON ON ON
I ON ON ON ON ON ON
      H
 0)
r-l

•8
H
   0)
   tot

   cd
td
                   ! A!
   w
  •H
  Q
           ooooooooooooooooooooooooooooooo
                  c
                  o
                  •H ,<—N
               JH U
               Q) cd ,
               4J O,
               cd -H-
              o
              rH

             !CM
             ' co
                                  o
                                  rH
                                PH  X
                                              o
                                              rH
                                           P^ X




                                              CM
                       m
                        o
                      ^
                      Z CM
                                                             —iOOoO
-------
                  0)
                  60
                  Vl CO
                  cd 3
                  43 4J
                  o cd
                  CO 4J
                  •H C/D
                  o
            NNHHMHHHHHHHl-IHI-IHHHHHHQQH
                                                                   T3  0)
                                                                    <1)  4J
                                                                   i—i  cd
                                                                    O  H
                                                                    >~> O
                                                                    CJ  (X
                                                                    a)  cd
                                                                    M  >

                                                                    co
                                                                   •rH  U
 Q)
r-t

•3
H
    O


    H-0

    o m
    n m
   Pk O
/— \
tJ
a>
H
•H
4J
C
O
o

EH

O
H
f*S
e
»-3
4J 0)
Gr-H
0) O
rH O
0) 0)
PH p^


                  0)
      tq
 q> crt y
4J43^«

tS CO r-H

   Q
   G
   O
               (U
                  4-> bC
                          ooooooLnoooor^oooi-icooocoooocvir-^
                          U1 O O
                                               ON\OrH|-^r-H C3
                                                   cd o
                                                   J-i O

                                                      CO
                                                   
-------
in
 i
      s
      E-i
       c:
 c     a)
 o     0
•H    4-1
4J  co  cd
 cd 'O  Q.)

 CU  Q) H
 D< O
O  Q) 4-1
       at
                     «
               •H 4J
               0 cd C
               HJd O
               O H «iH"
                     O
                     CO
            0)
            bO
            J-i co
            cd 3
            Xl 4.J
            O 03
            co 4J
            •H C/D
            Q
            C!
            O J-l
            •H >•

            0,0
            OM--J
            ^M-l
            P-i O
                           W Q Q
                           CslNIISlQl-lQMHQHQ M H  QHMQQHHHMQQQ^
                                                                           f --- :tOOi— ICXJOOOOO
                                                                                                            00
                                                                                                            C
                                                                                                           •H
                                                                                                     Q

                                                                                                     co

                                                                                                     §
                                                                                                     (!)
                                                                                                     a

                                                                                                     Q
                                                                                                            o
                                                                                                           •!-f
                                                                                                            CO
                                                                                                            3
                                                                                                            M
                                                                                                            4J
                                                                                                            co
                                                                                                            C
                                                                                                            cd
                                                                                                            (U
                                                                                                            e

                                                                                                           w
                                                                                                      60
                                                                                                      C
                                                                                                     ••-I
                                                CM    vococMincMcoo   r-~.inr-»oooovo
i-4
o
C/)
    4-1 (U

    3'OOOOOO-3'
-------
             0)
             60

             td
                     M
                  o cd
                  M 4J
                  •H CO
                  Q
                          NNNINIHMQH1-IM
      H
      !S
      13
            O M
            •H >,

            0,0

            13
            O «W
            MM-I
            PM O
                          voo^ooomo
                          mcMinoooooo
oooinooi—icoo
VOCOVOCNJOOOVOO

i—toovovovovo  r—3"
      r-100    rH  r-I^J-
                                                    O
                                                    O
                                                    ON
vD
 Q)
      H
§
M


I
CO

CO
CO
3
£
la
o
H
CO

§
H
            4J (])

            0) O
            o >-
            M O
            0) (1)
               
-------
0)
60'
M
cfl
     CO
  o ti
  M 4J
  •H CO
  0
           H H Q H H
  O M
  •H H

  q ja
  PM  o
         o o oo o
         O O iT> O
         C5 P^* ON iO

         in rH i-H i-H
         
0)
I-l
,0
cd
H
^-^
H

pQ

.O
S3
H
W
d

w
IS
JJ! (1)
CrH
OJi O
0 !>,
5-1 O

-------
 d>
 60

 cd
                    CO
                 O cd
                 CO 4-1
                 •H CO
                 Q
                          H P Q Q H H
                 O M



                 0,0
         O O OOO O O
         O O O COOO
         CO OJ O C7\ O in

          O O <1" 00
         co o** *xi* c^j *s^ vo
                                         ~,
I-l O
                          O O
 0)
 cd
H
CD
01.  .
I-l M
             •^~  ^
              cd  co
                         o o o o o
                         o m cr> co o
                         i—I CO CO CO<}-
                         CN Csl
                                      00
a
o
             .2.0^

             Cd i-l rH
         O O OO O O
         O tr>  cN O CO
         rH COOOOO  0)
                ens
                cd  o
                r-l O
        O] vo vO r^« xd" vO ON in
        r-IOO-cfOOOcM
                                                                                                                  a)
                                                                                                                  4J
                                                                                                                  o
                                                         92

-------
  0)
  60
  5-1  CO


  "O  oJ
  CO  4-1
  •rl  CO
  O
                     M
                          SISISISISISISISISIQMQHMHQl-IHClQQQMHQMQQ
             O rl
             •rl >-


             "rQ
              O M-l
              5-1 M-l
             PH O
         CMr-IONoOOOOOOOOOOOOOOOvOOOOONOOvOOOl^-Or-»
         rHCMCMcMOOOOOOOOOONOOONvOVOOOr^OOOOcMCMOt—loo
                  SOOOOOOOOOoOOOincMinOOt—loOONvOt-l^fl^vO
          cMON vo r-- oo oo
            tH   OO
CM oo oo o oo in o
   t-l CM vO OO    i—I
          CM
-3-oooooNinvo

 0)
r-l

•3
H
   V O
   o >•
   5-1 O
   Q) Q)
  PM p4
5-1  5-1 6C|
0)  cd ,
           Cd
              M
             •t"1
             O
                     oooooooooooo
                     ooooooooooom
                     rHr-lr-IrHt—It—It—It—It—lr-lt—I
                 !cooooovooi^r-i
                 ; ON         moo    m vo
                                                                                   ;o o o ooo
                                       vo vo
                     ooooooooooo-
                  . r-~OOcM
-------
                    0)
                    00
                    J-)  CO
                    cd  3

                   •ss
                    CO 4J
                   •H OT
             M H
                         HHQQQQHHQMHQH
                   'Q
                   OM-1
                   j-im
                   PM O
         O CM O
         O CO 
         O--i  M 00
                
                   C'O
                   Ctt  O
                  r-(0
                  PM
                             100
                             100
                              O ON
                                ^  »\
                              i-i m
                              CM CO
         CM 1^- rH in OO CO <}• CM CO
                                                            CO
                                                OO
         COCOcMOr-ICMCMCOcOCO
-------
                  0)
                  00
                     CO
                  o cd
                  CO 4J
                  •H CO
                  O M
                  •H
                  4J ---
                  0,0
                  O M-)
                  j-i M-i
                  P-i O
                           OOOCMOOOOOCMOtnOOOr-ICMOCOO
           oo
                                                                       r-HOOOOOOOOoO
                                                                        i
                                                                                     l CM
                  4J  0)
                  CrH
                  
                   !£
i ON ON
; ON ON
i*
I ON
,   >ON
;ONCN
                                                    jr^OOOOOOO
                                                    ;r->-ooooooo
 Q)
r-<
^
 cS
H
      !25
a)
                   co
                  •H
                  Q
                                                                        oo

                                                                        C--'i—I  O

OOOOOOOOOOOOOOOOOOOOOOO^OrHCMvOvOr^r^-

                                                                                          00
   G
   o
   •Hx
}-l -U 00
CU «fl ^s5
4J O^
CS •!-!--.
S 1-1 r-l
   tt^-^

   £
                              o
                             ' CM
                                    vO
                                                      O
                                                      CN
                                                     loo
                                                     ;   "
                                                      oo
                                                                                 o o
                                                                                  x x
                                                                                        !
                                                                                  r-- CM
                                                                                  oo <^
                                                                                   •  •
                                                                                  CO CO
                                                                                          O
                                                                                       O r-l
                                                                               00
                                                                               m CM
                                                                                   •

                                                                                  CM
                                                                                                         0>
                                                                                                         4J
                                                                                                         H
                                                                                                         O
                                                                                                         o
                                                                                                         G
                   ct! O
         irir^r^oooo^r^cor^ovOi-i^i-o-cJ-cOcoco^t-co^LricMcOfovo^Toor^
         OOOOOOOOOr-ioOOOrHOOoOoOoOi-iOoOOOOO
         o^CMOCMCMCOO<^>CyNCMr^OcO"^r-lOO
-------
                  0)
                  00
                  M  ca
                  cd  3
                 ,a  w
                  o  cd
                  CO  4->
                 i-l  W
                 Q
            SISIS1S1S1SIHQHQHHQOHQHHQQQQQQQQQH
                  O  M
                  0,0

                 *o
                  o IH
                  p i| |
                 PM  O
           OOOOOOOOr-»OOOl	^OOON^OOolOvOOOO
           ooooocooovoooor-^oooocMoooOinoinooo
           OOOOOvOOOONOOOcOOlOO-tfOO inOONOvOOOO

           ooooocNoooooin     o

 0)    H
                  -O  0)
                  Ci-H
                  Q)  O
                  O  £~
                  >-l  O
                  0)  Q)
                 P-i P4
                  Q)



                  ct) Lv(



                  CQt-1
                 *r^
                 Q
                               in oo o in >

           ooooooocor-i—icooNininoNoooNco
                                  r-HCOoOCOini^-CMOOr--
                                                    i-l CM CO CO
n
0)
4J
                  (3
                  o
                 •Hx-s
                :iHi-l
                 m
00! « i i' | ^ (,>j ". >i c j v i ^
                                  i—i oo co O co >>o i—ivo oo
-------
                  QJ    :
                  &0
                  M  CO
                  cct  0
                 JS  4J
                  O  cd
                  CO  4J
                 •rl  CO
                 O
                                                                       Q Q QQOMOHQQ
                  CS/-S
                  O
                          mOCMOOOOOOOOi-iinOOvOOOOOvOiN O^O

                                OOOOmOOOinmOOCMONONOrHCOOOOXl-CMO
                                                                                oo.d-oOvovoooo
                                                                               - oo rH °irrI~
0)
-U
Vj M
«JjSd
^3^!
CJ-^
CQr-l
•rl
O
                       o<- i ocoooi-io  i ooofoooooo  i
                                 fs. '      in       co      ON                co <^> <*Xc»,
                     000 00 00 00 00 00 00 00 00 00 00 00 00
                     _i_i_i_i—j.-j,— (i— li— li— Hi— 4r-lt—r-lr-i!— I i— II— i i— ( i— i rH I— I i— ir-lr-li  I i— I
                                                           ' «— ii— i
                   C
                   O
                a)
                4J
                cfl
                   4J bO
                       CM CM
                        oo
                        rH i-l
                      4  X  X
                      5 CM r-<
                        VO CM
                    CO CM CM CO
                     O OO O
                     i—I i—I i—I rH
                   4  X  X  X  X
 CO CO CO CO 
  OO rH O^i O"» vO i—1
  O 1^ rH rH OO O
                                                          COCOCOCOCOCOCOCOCO
                                                           ooooooooo
                                                           r-lr-lr-lr-li—li—li—li—li—I
                                                          dXXXXXXXXX
                                                        \O CT* CM O in O O CO CT*
                                                        co
-------
                    0)
                    60
                    !-l  CO


                   ,£ 4J

                    O  cd
                    CO 4J
                   •r4 CO
                   Q
                      QHMHQHQQMHHQQHHN1N1M
             O ^
             •H £-

             0,0

             £^
             om

             PM o
                            OOOOOOOcOcM-sfOf^OvOoOOOO

                            OOOOOOOOoivoovOO^OOOOO
                            t~*l ("™* (*"> ("^» ^"^ !*"» *^% /~\ ^-^ ^-t" <•••* /^\ ?"S «»J l«*^ <•••»* /—N *—\
                            r~- vo
                                        m CM

                                        r>» CM i
                                                O CM


                                                CM
 0)


I
 o
o
CM
iH
 I


 0)
t-J

•s
H
w
g
s

1
H
PL,
   4J  0)
   Cr-l
   0)  O
   o  >.
   M  O
   0)  0)
             0)
M
0)
4J
cd
                w}
              ! A!
ooooo

ooooo
ooooo

OOOOOI
000
  • O CO
O rH i-H
                    co co co co n in
                     ooooooooooooooo
                           i — d'
             c
             o
            •r4s~«
          M 4->  6C
          Q)  cd, •
          11  rj
          rt-H-
                              ooooo   ooooo
                        mi	CfOO    CMinOrH
-------
                0)
                bQ
                rl CO
                ed 3

                O cd
                to 4J
                •rl CO
                Q
            OHM
                O  rl



                0,0
                 O M-t
                 rl 'W
                p [  O
                           • vo
            ^00 rH
            vo r~- oo
            rH O>00
CO
   4J  Q)


   (U  O
   O  >i
   rl  O
   0)  0)
   Pq pj^
                          O O O
 0)
1— I

•3
H
    0)


 r-~
             CM O O
             rH v£> VO
             r-l OO
                                                                                                                       CD
                                                                                                                       4J
                                                                                                                       O
                                                              99

-------
                                                                                                              •*   CM
                                                                                                              O   O
                                                                                                              O OO OO
                                                                                                              O O O OO    OO
                                                                                                                                       00
                                                                                                                                       000
                                                                                                                                                                o
                   o
                   CM
                            60
                            B  m
                                                                 OOOOOOOPIrHV
                                                                                                                  O.VD      m          rt
                                                                                                                  CM CM      OO>O\    O
                                                                                                     (OOOCOOOO    Oi-(r-lOOO

                                                                                                                             d ddddd
 I
>
                        toi-i  co
                        a>i-i  ta
                        MO*
                                                                                                                             O CM CM O O O

                                                                                                                                   rt odd
                  o
                  «n
                  OJ
60
B ,
•H 0)
y 1-1
(S05


i-i
a
Q


ton o
CM CM C\
VO



OOOOOOO
CJ^OrHinO O
rH ONO
•*

<)• rH
r^-cM
dd

                                                                                                  o

                                                                                                  d
                                                                                                                 00

                                                                                                                 do
                                                                                                  o

                                                                                                  d
                                    o

                                    d
     ooooo

     ddddd
       0)  60
       B  B  01
<*1    1-1 iH  CO

S    -3§.g
          4>B5
               (MOO
VDCO OS
      CM
                                                                                                                                    1-1   m
                                                                                                                                    o   o
                                                                                                                                  oo   o
                                                        COOOCMOO
                                                        f-l       V
                                                                                                        OO
                                                                                                                 O
                                                                                                                 V
                                                                                                                         o

                                                                                                                         d
                                                                                                                               00
                                                                                                                               ooooo
                                                                                                                                                         ooooo
                                                                                                                                                         V V
                 VO
                 VO
                 CM
 60
•H  M
»-<  O
 ta j->
 09  «

r
                                                                                                       o

                                                                                                       d
                                                                                        o

                                                                                        d
                                                     o
                                              Ur-l 4J
                2
                u
                •J
                w
                           co
                          •a
                          iH
                        BrH
                        o  o
                       J3 W

                        WO
                       O  O>

                        O  B
                     COiH  01
                  ra  3  e  ft,
                  0)  U  (8  CO !
                                                         B
                                                         01
                                                        1-H
                                                         CO
                                                     rH  >
                                                      Q  at
                                                     •u  x
                                                             0,0
                                                                               B  B  at
                                                                                                          Ct)
                                                                                                          4J
                                                                    ai
                                                                    co           -
                                                                    ai          co
                                                                    B rH     prH
                                                                    Co 0)     0)  O
                                                                    eo^ii  u  >  c
                        B  0)  01  01
   01                  iH  4J  4J  U
   B             01     0  CO1  OJ  m    0)
 -CO       0)    *O     COi-HrHrHflJ4J
   450)    B    i-l    rHCOcHCOJJCD
   .UB    0)     tt     (3J2jIIJ3COrH
   O)CO    p     O     O>4J4J4_lrHC(]
0) O X   rH    rH    J3X!J3jEC8X!
B )H iJ    O  01J5   .  D, O, O^Oj xl 4J
0)00)   .U  C O  O) iH rH rH    4J 43
N rH p a  o  oi     c -a  x  :    •  - -
B43(J»HrlNO)0)OO)N.
0>VO.04JBBrHC043B4J
                                                                                                                                                               0)

                                                                                                                                                               01
                                                                                                                                             JJ
                                                                                                                                           0) 0>
                                                                                                                                           B O
                                                                                                                                       0)  0) U
                                                                                                                                       B  IH O
                                                                                                            N O  I  BOO
                                                                                                                                      ^ W
                                                                                                                                                   0)
                                                                                                                                                   S
                                                                                                                                                   01
                0)
                S
                                                                                 100

-------
•o

 I
 c
 o
60 .
•5.C
CM r-l JJ
in ^ cd
CM O «
OH

JJ
60 B
JJ C td
i-i e jJi-i o
r-l d) Or-l 1-1
CM o.rcrH u
V* O .O
OS 3
rJ

•D
0) 0)
r-l JJ >,JJ
1-4 td I— I CO

£°*
60
i-t ai
r- r-i to
O Jx! S
CM O «rl
s^

B JJ
O B
--1 a
co JJ jj a
r-i 3 td JJ
CM r-l O td
o S3 a)
CO 1-4
H
60
r~- i— i a
CM C8 JJ
CM a) ed
BS
B
i_)
cd
Q


r-l
.,,
cd
a



r-i
^
td
o

>N
OS
0

r-l
•j.
0)
Q



f>

C

co  OO O O O CM r-lO OOONO O O OO O
<*• in r^ m
r^t
oo in i— i
o 
a> o B to
ffiffi r4 H S Cd
Cu B. 3 < fl)
CO
•o
BrH
,E£
^1
cd TJ
o a)
•a
0 B
coi-i a>
co 3 B 0.
Q) )J 0} CO >>
                                                                                  4J
                                                                                  C
                                                                                  0)
                                                                               I-l  >
                                                                               2.S
                                                                                                          cs
                                                                                                          jj
                                                                                                          o
           ai

           cd
           J3
           jj
           a>
         a) o
         B M
         ai o
                                                                                                                              ai
                                                                                                                             •o
                                                                        Vl
                                                                        o
                                                                              01  0]
                                                                              4J J-l
                                                                              CIS  Ct)
                                                                             r-l r-l  8)
                                                                              cd  cd  JJ
                                                                                                                        jjcua)r-i
a>
to
a>
BrH
<0  0>
OOjxi
      OCO
      3O
      -ij:
0 O faOlHH«OOU
    -    OIOO4JCBr-lj2JJ
   roo).2i-iu-ii-Ja>ci>aJrv>3'-iO
,jrHC30VHOCSJ3r-lj3japQ>,c8
cuoaiuHt-ij-ir-i >,JJ  JJ  i
>  C  N  O  I  O O
                                                                                            JJ
                                                                                         oi ai
                                                                                         B o
                                                                                         ai to
                                                                                            o
                                                                                                                                                        a)

                                                                                                                                                        a)
                                                                                         4J.c
                                                                                         CCJ
                                                                                         « to
   
   o

01  o
BI-I
01 J3
                                                                                   101

-------
                60


               •5.C
                UK)

               Ck
                        a
                        a
          _
          OOOO   OOOCMITICOO OOO-tfvO

          oooo   oooot-Ht-HO dddi-3 PI
                       eot/i               ovOr-t    \6
                                           o   rH
                                           ooo ooo
                                                                                           o
                                                                 o

                                                                 d
                                                                                 00
                                                                                   •  •
                                                                                 oo
                                                             o

                                                             o
                                     o

                                     o
oo ooo

do odd




rf*"S
*0
§
c
*ri

B
a
Xw*
•*
»-l
1
&
r™^
JO
Q
1-4











CM
CO
•«•
f«»
•*

g
s










,
1-1
CM





O
CM
i-l




§
<•



JJ
B B
•S JJ 1
jj a jj
3 oi a
i-l S 0
0 14
W H


1-1
^
0





0)
O M
05 ti O
J£ 3 JJ
^W*

1-4

a
o

•O *O JJ
oi o> o
B JJ 0)
•H a 3
Jflli-H
MU-I
H>M
W


i-i
>,

Q

                                                                                                                      OO

                                                                                                                      do
                                                                                                              o
                                                                                                               •
                                                                                                              o
                                                                                                ooooo

                                                                                                do odd
                                                                                                     oooooooooooooooooooo
                                                                                          fOOOOOO   O

                                                                                          dpdddd   d
                                                                                          oo

                                                                                          do
                                                                                                                              O O
                                                                                                                              00
                                                                                                                              oo
                                                                                                                              V V
                                                                                                             o
                                                                                                             o
                                                                                               oo
                                                                                               ooooo
                                                                                                                   ooooo
                                                                                                                   V  V
            (XO)  U
                    13
> B  CO       OB
< H  a    t»-<-i CD
 <  0)  m 3 B O,
    jj  o) (4 a ca  >>
 jj

 B
 01
 !-<


.?
                                    B
                                         -
0,0
                            0-
                            B B ^J a a  S

                                 ^S SSI'S
                                                           e
                                 0) C r-l
   0)
   B


  J3  0)
  JJ  B
   01  a
   O J3 •
01  W JJ
BOO)
0)1-4  O
                                                                B   «^
                                                                OJ    H
                                                                3    O
                                                               • 1-1 •   I-H
                                                                o q> JG
                                                                4J C U
                                                                P «
                                                                                                                           B 0)  0)  01 0)
                                                                                                                           •rl JJ  JJ JJ JJ
                                                                                                                           s a  a  a a
                                                                                                                                            01
                                                                                                                           B J3w3 J3J3 ar-t
                                                                                                                           01 JJ jj jj jj f-i  cd
                                                                                                                          js~js ja tc Jd a js
                                                                                                                           a, ex CL.O-I K f jj
                                                                                                                                        JJj
                                                                                            B-OX
                                                                        0) O O  O JJ B
                                                                                         Br-l  ra J2
                                                                                            a  o
                                                                                                                        0)
                                                                                                                        B
                                                                                                                        0)
                                                                                  JJ
                                                                               0) 0)
                                                                               B O
                                                                             0) o> h
                                                                             6 P. O
                                                                                                                                                          0)
                                                                                                                                                          B
                                                                                                                                                          01
                                                                                                                             0)
                                                                                                                             o
                                                                                                              J3 0) O
                                                                                                               O Bi-H
                                                                                                               a oi x!
                                                                                                               U 3 U
                                                                                                              Jjl-l 1-1
                                                                                                               01 O rJ
                                                                                                              HHH
                                                                    102

-------
                 CM rH
                                                                                                                                     CM
                                                                                                                                     1-1 in m ooo

                                                                                                                                     o CM CM ooo
                             •O
                              0>  >N«>
                              JJrH W
                                S.H (0
                                O «J
                                                                                                mr~-          cMin
                                                                                               

 0
r-l
XI


         <0 JJ

        I*
                                 60
                                 s
                  	    C^Or-l OJ
                  O J3 CO CO e A! C
                  CM  B A! 41 « t> •«•<
                      OrH i-l    i-l|3j
                     CJ<5 O    CW
•O
 o
D  tO
ca
                                                                                                                              o

                                                                                                                              d
                                                                                                                                 O

                                                                                                                                 d
                                                                                                                  o

                                                                                                                  d
                                                                                                                  oo

                                                                                                                  do
                                                                                                                       o

                                                                                                                       d
                                                                                                          o

                                                                                                          d
                         ooooo

                         dd odd

CO
CM
CM



0) 60
e e 01
i-l 1-1 03
r-l C C
co a 1-1
X & t6
rH r-l
^J O
CM

*
CO
C)


OrxO
• • •
p*^ oo cr*
C*J



                                                                                                                IT1CO   r-l
                                                                                                                00   O
                                                                                                          i—I O OO OO
                                                              CM OOP") ON OO
                                                                                                               oo

                                                                                                               dd
                                                                                                                           o
                                                                                                                           o
                                                                                                                                    O    OOOOO

                                                                                                                                    d.   dd doo
                                  .60
                  \o
                  cs
                  CM
                                    in in
                                    oo   -*•*
                                                                   m                   
                                                                   vo in          m    o
                                                                    ")rHOOOCMOO

                                                                     i do o o oo o
                                                                                                                               o

                                                                                                                               d
                                                                                                                   o

                                                                                                                   d
                                                             O
                                                            r-l
                   H
                   •z.
                   r-l

                   2
              0)    <>

              0M    CO
                                                                           ra
                                                                           •O
                                    _          Cr-l
                                    S          o o
                                               J3 CO
                                     O          rJ
                              Or-l 4J          CO *O
                             OB)            CJ 0)
                                 JJ  • QJ         *O
                               ai o  B to       u c
                        B333rJHScO    mi-14)
                         0.0,3    <s 9MH f—* .CvUE't-IW**-!*]-!
                               s H u o o C&£H«OUCJ
                                                                                                                          c a) « a)
                                                                                                                         i-l 4J 4J 4J
                                                                                                                            co co co    01
                                                                                                                            r-l r-l r-l 0) 4J
                                                                                                                         I—I tO CO <4 4J CO
                                                                                                                                     COrH
                                                                                                                          21 4J JJ 4J r-l
                                                                                                                                  £
                                                                                                                            a. O.BL4 js
                                                                                  103

-------
                               JJ
                            60 e
                      JJ    C S)
                  rH C 4J1-) U
                  rH 4) OrH i-l
                  CM G-S-H !J
                      CO    C J3
                           Bi 3;
                                                                                       CM -3-
                                                                                    CO    mrH   i-< CO
                                                                                    ON    o o   o o
                                                                                    OOOOOOO
                                                    in in t-li-l
                                                    oo oo
                                              oooooo
                                                                                                                                 mm    rHrH
                                                                                                                                    §O    oo
                                                                                                                                    oo o o
                         •o
                         0*
                               0)
•o
 o
I
 i
>.
      CM
      CO
      •a-
                         BJi-l CO
                         Ol^l 03
                         uo*
       C     JJ
       o     c
      i-4 JJ  fl)
co    a «  a
f«     3 01  JJ
CM    rH K  13
       O     U
      CO     H
            H
                                     CM
                                    CM
                                                                                                   rH CM          mmrHrH    mm       rH
                                                                                          _       oo          oooo    oo       o
                                                                                   > o o o o o o o.   oooooo    ooooo

                                                                                                                                 ooooo
                                          co coo

                                          mmco
                                                                                                                  r-< m    I-H
                                                                                                                  oo    o
                                                                                                               ooo    o
                                                                  oo    o
                                                                  ooooo
                                                                                                                                                   ooooo
                                                                                                                                                   V V
o
CM
to
e
i-i cu
fH CO

U 1-1



CM

^,
S)
Q


rHCM O

CM CM CO
m

                                                                                                                                                   ooooo
                                                                                                                                                   ooo oo
                  VO
                  o
                  CM
          60
          C  0)
         1-1  CO
         rH  C
         Jrfl-l
                                          CO-* O
                                                                  OOOOO

                                                                  ddddd
                  CM
                  CM
                           60
                           <3 JJ
                           a) a
                                                   mm
                                                   OO
                                          OcMOOOOrHi-4l
                                                                                         m
                                                                    CO CO               O
                                                                      > i-lOOO r-lO O
                                                                                                     o

                                                                                                     o
                                                o
                                                o
            &>
            C3
           Cu
                 s
                 1-1
                 CM
                 CO
                                    ij             co
                                    o            -a
                                    rH            i-J
                                    J2          OrH
                                    O          O O
                                               JD CO

                              OtH JJ          (-CO
                             O   (8            CJ 01
                                 JJ  • fl)         "O
                              4> o e co       u e
                       S E !JH B rt    ca-HO)
                        O.&.3    < <1) m 3 C Cu
   JJ
   e
   01
   rH
   St
rH >
 SI S)



II
                                                                                 Eg
                                .ee     ora
                        ex  Bwsii-ijso
                           (d  0) >• >M-1 tHJ3
                                                      E  e-   e  E
                                                OOCP«j2ji
               01
               CO
               0)
               CrH
               CO 01
               BOJ
                                                                                                      M
                                                                                                      O 4J
                                                                                                            N  4)
                                                                                                                    4)
                                                                                                                              B  CrH JS JJ
                                                                                                            *   fl)CJ___.       ,	 ^
                                                                                                            CO  41J3.HIM.H 4) 4J'cO >,3rH r . ,
                                                                                                        MrH  C 0>j O CJ01-IJ2J3W >,£ CS

                                                                                                      o >  e  to o  '  o o >ijr js w 2; jj 41 js
                                                                                                      CrHOlCrHrHrHlJJjJCljl   I  CDEJJ
                                                                                                            -141jSrHJ-VOjJ4)(|JCMH-)i-li-l
                                                                                                                                                           41
                                                                                                                                            01

                                                                                                                                            2
                                                                                                                                      .    .  o
                                                                                                                                   B U  B rH
                                                                                                                                   ra ra  oj jn
                                                                                                                                   B (J  3  O
                                                                                                                                   4) JJ rH «H
                                                                                                                                            tJ
                                                                            304

-------
•e

 2

 c
ft    ts
 4J    CO
 e    -3-
o
o
•O    4J
 £•« a
 e oi a>
•3 u s

 s OIM-I
                                       000
                                                                    CM i-l
                                                                            CO

                                                                            04
                                                             CMrH
     O-    CO

     VO    O

OOOOOO


LOOOOOO
OJ
           o
        oo
                                                                                                                               oo
                                                                                                                      o
                                                                                                                      o
                                                                                                                                       o
                                                                                                                                       V
                                              o
                                              o
                                                                                                                                      o
                                                                                                                                      V
oo
ooo  oo
                                 ooo oo
                                 \f V
I
•o
01
o c
Oi-l
^•8
o
0


oo
o
0)


4J
60 G
e a)
ft 01 B
i-H *J 4J
U B 01
•t"J ^ Vj
fc H
60
c o>
i-l 09
r-l C

U BJ
OH

W

>
B
Q



CM

>i
cd
Q

                                                                                                         in
                                                                                                         O
                                   O O   i-i oi\O            O_
                           OOOOOO-*"^OOOOOi-iOOflOOOi-iroOO>rtOOOOO
O


d
                                                                           r-
                                                                           ro
                                                                                OOCM VOO<-I
ui
!>-<

c4ooo oo
                                                                                                                          o

                                                                                                                          d
                            00

                            do
                                                                                                                   00

                                                                                                                   do
                                                                                                                                       o
                                                                                                                                       o
                           O
                           o
                                    o

                                    o
                            o
                             •
                            o
                                                    000
                                                    ooo oo
                                                                                                                                                          ea       o
                                                                                                                                                        V  V
                                                                                                                                       o o o o o

                                                                                                                                       d d o d d-
                 o
                 CM
                          0) H

                        0) O 0)
                                   OO   csl 0s
                           OOOOOO>-iOOOOOOOOO<-iOOO

                                                                "dodddo
                                                                                                         f>CM    CO

                                                                                                    ON   OO    O
                                                                                                                                        oo
                  2
                                                                                                                                                 0>
                                                                                                                                      C  0) 0) 0)  4-1
                                                                                                                                     i-l 4J 4J J-l  B

                                                                                                                                      B. B B B r-l
                                                                                                                                              -I  B

                                                                                                                                         B B B J3
vo    td


 0)    p r




CM    CO
                                           B O>
                                        S S H O OOt*
                                                                        105

-------
                          60    B
                          cum
                   COtJ -rl  C  O
                                  i
                   CM  OF-)  O.U
                      O  OCOXl
                         CJ     P
                               t4l
                                         in tr>

                                         ooo

                                         odd
                                         V V CM
                                               CM
                                                                    OO OlOrOCO
                                                                                                               co
                                                                                                   o\          o
                                                                                                   OOVO VOO O O
                          -3-OOOOO
                          CMCM
                          cMr-.
                          i-l CO
                          VO
                            •* CT> i-l O irt CO O (
                            to CM       i-l VO
         >i- 3
                                                                      CO
                                                                     •a
                                                       O O
                                                       J3 CO
                                                       rl
                                                       (S T3
                                                       O (I)
o
00
81
                         O B
                      COi-l (I)
                a) co 3 B a.
       -        lJfl)r|C8cO>>

    §S  rfO-D   *^ ° ^°" 5
    a  fllfl'rl
t-l t-l  D.C  C    O
 B  X  B  CO  COrH 3
1-1  O  fl)  X >,Tl 1-4
SSHOOOfa
                                                                                     (8
                                                                                 i-l >
                                                                                  (0 C(J
                                                                                 4J X
                                                                                  O  B M
01
B
s)
x; a)
; jj c
fl) «
a) ox;
B VJ 4J
0) O fl)
N r-l O

CD O O
X> t-l r-l
O UXi
MHO
O 1 CO


0)
B
0)
3
I-l
o
JJ
E O

O 4-J
IM •*-(
o c
o o
                                                                                                                       fl) .C
                                                                                B  (1)  fl)  fl)  fl)
                                                                               f-4 iJ OJ 4J 4J
                                                                                e  to  ro  to  to     o
                                                                                Ctf i— I rH fH i-H  fl) 4J
                                                                               i-icDcscdctlajnj
                                                                                C .£! J5 J3 J2  « r-l
                                                                                0) 4-1 iJ U 4-) r-l  Id
                                                                               Xx^^BrCXIcOvB
                                                                                O, CX CXCU Ck J3 4J
                                                                                                                                                         fl)  01
                                                                                                                                                         CO
                                                                         .
                                                                   JJBODfJ.r-li-1
                                                                      CD    B -D X  fM-l i-l X! P<  CD  0)  rl
                                                                      HO)CDOCUN>^ XOj     B  rl  O
                                                                                                                                                                  0)
                                                                                                                                                                  O
                                                                                                                                                                  rl
                                                                                                                                     va)cji-io4JXa)o
                                                                                                                                rixixipao  >>xl a)  B  o  a r-i
                                                                                                                                               X! U h  Cd  CO  0) X!
                                                                                                                _ .   r-l  « r-l  I XI -0  0,3  I   4J
                                                                                                                a) x! f  fl> xi'"     "  ~'  "  ""   '
                                                                                                                                                       SoJCDXIBriSO
                                                                                                                                                                    0) 4J rH 
-------
               00
               1-4
               CM
                     B   AJ
                     o    B
                     "•"    2
                     u u  8
                     a cd *j
                     i-< 0)  Cd
                     o s  

 01
rH

•8
H
CM
CO
4J
B B
o a)
U Cd 4J
r-i 53 0>
O >-i
CO H
60
B 0)
ft CO
rH B
U B*
O,

co
£
0


CO
cd
Q

o-
eyioo o rHOOOOo
r~oo
tf
3NOOO
   s
              ed    <
              P*    W
                                                                             107

-------
                      41  ra
                     r-l  O
                     vJ. T4    .M
                  o\ .u  B O.B
                                                                                                      •*    CN
                                                                                                      O    O
                                                                                                      oo oo o
                                                                                                       o
                                                                                                       o
                                                                                                       to
                                                                                                       IN
                                                                                                                OO OO O
                                                                                                                       oo
                                                                                                                       do
                                                                                                                                                                   OO
                                                                                                                                                                   oo o
                                                                                                                                                         oo o
            jj
      •O-O B
       QJ  Q) d)
       B JJ 3
O    M  Br-4
O    J3  (!) UJ.

                 CM e  o  co  c
                     O— I  C3  0)
                                                                                                       •*    v
                                                                                                                         oo

                                                                                                                         do
                                                                                                                                  o
                                                                                                                                  o
                                                                                          o
                                                                                          o
                                                                                                                                             oo
                                                                                                                                             oo oo o
                                                                                                                                                   OOOOO
                                                                                                                                                   v v
4J
                        0)    M
                 O     U 0) 01
                 CM     M .M 4J
                        D 05 C
                       CO
                        CO

                         >,
             jj
       B    B
       O    V
      •rl JJ  B
       JJ     CuO M
      CO M J2
                                    O

                                    O

                                    oo
                                                                  ITl
                                                       _         O
                                                    oooooo
                                                                                     COCsJ IAOO
                                                              "•X/1OOOO
                                                              \OCM
                                                                        CM ON r-l O M
                                                                        !-.
                                                                        CO
                                              •*    CNVO
                                              vB    O O
                                        OOi-HOOO   O

                                        J
                                                                               JJ
                                                                               B
                                                                               0)
                                                                               i-l
                                                                               as
                                                                            "> >
                                                                            as as
                                                                            B B
                                                                                                    0)
                                                                                                    B
                                                                                                    cd
                                                                                                    J2 0)
                                                                                                    •U B
                                                                                                    01 (0
                                                                                                 01 OJ=
                                                                                                 B M JJ
                                                                                                 0) O 01
                                                                                                           01
                                                                                                           a
                                                                                                           01
                                                                                                                 01
                                                                                                                •o
                                                                                                                         I-l
                                                                                                                         o
      B 01  0)  01  0)
      •H JJ  JJ JJ JJ
      B >
                                                                                                                                            ,	a)  
-------
•0)
     £
-n   £

T   £
>•    •*


     §I
     MOO
.0   JO!
 <8   Pu
E-1   S
cS
                  0) CO

                 1-1 O
                 H-l f-l   Jt
                 *J B O.S
               ON a) 
                                                                                      eg
                                                                                      4J
                                                                                      O
                                                   >>
                                                   c
                                                   oi
                                            CuO   E
                                          o«>   i-i^.
                                          3OJ.i4-i-urai3MVia.ot8
                                   Br-4
                                   « 0)
                                          MrH B
                                                                                              0



                                                                                              4J
                                                                                              0
                                                                                              O
                                                                                              u

                                                                                             i^e

                                                                                             '•SS
                                                                                                     U
                                                                                                     4J

                                                                                                     rH  0
                                                                                                     «  U
                                                                                                        a
                                                                                              000
                                                                                              BrH.fi -
  0


  0
0 0
a o
                                                                                                          e  1-1 o
                                                  -
                                        o > a S o  >
                                                                                         B*-i-li-liT.l
                                                                                                             >.C8
                                                                                                             £h
                                                                                                             UJS
                                                                                                           I  0 4J
       0
       B
       0
       4J
       0
       O
                                                                        B O Brj
                                                                  109

-------
      I
      §
I
 e
3
U1   MOO
T4   J^**

>   5
 as   co
r-4
X)   tu
>«


I
CO
             o
             CO
        a
        ft.!! r-l
       1-100)
        O rJ 4J
       i-l 3 O
                                                        o
                  §
                               U
                          to    e
                          cum
                      4J«ri  C  O
                   «
O U *r< B O
O O M O> i-l
CO E3M &,»•)
O WX1
OS 3

01
«
Q

                                            U1VOC4
                                                  CM
CQP1O

     >c-3
      01
                                                           OOOOiOOOOOOrHOOOOfOOOOOO
                                                           •^*       vo r^
                                                                                                                          o
                                                                                                                          d
                                                                                                                        oo
                                                                                                                        oo
                                                                                                                       oo
                                                                                                                       do
                                                                                                       O
                                                                                                       o
                                                                                                                                                             OO
                                                                                                                                                             oo
                                                                                                                                                                         OO OO
                                                                                                                                                                         O
                                                                                                                                                                ooooo
                                                                                                                                                   o
                                                                                                                                                   o
                                                                                                                                                            OO
                                                                                                                                                            V V
                                                                                                                                                      oo
                                                                                                                                                      oo
                                                                                                                                                                         oo
                                                                                                                                                      oo
                                                                                                                                                       V  V
                                                                                                                                                                     ooooo
                                                                                                                                                                     odd dd
       60    C
       qua
*-< t> i-l c  o
O Or-l tt)^

       o coxi
      os     9
                                      eoo m
                                                                                                                                         oo
                                                                                                                                         do
                                                                                                                                                  o
                                                                                                                                                  o
                                                                                                                                                      o
                                                                                                                                                      oo
                                                                                                                                                               ooooo
                                                                                                                                                            oo    ooo oo
                 s
                                                     .   o
                                                     03 jj
                                                     4J  -a)
                                                  01 o B to
                                           ffiSS  UH B OJ
                                            O.D, g    < a)
                                                  4J  •>    LJ
                         B r-l
                         O O
                        X) CO


                         WO
                        O 0)
                            •o
                         O B
                      09 >r-l 01
                   CO  3  B O.
                   fl)  r-l  ffl tO !
                                                                                       OJ
                                                                                       c
                                                                                       01
                                                                                       1-H
                                                                                       a
                                                                                   r-l >
                                                                                    ns e)
                                                                                   •U X
                                                                                                                td
                                                                                                                4J
                                                                                                                o
                                                                                                                H
                                                                 o.O
                                                                              B t-l
                                                                                       B
                                                                                              DO
                                                                                              01
                                                                                              Cr-4
                                                                                              CD 01
                                                                                              WJ.M
                                                                                              c o
   01

   ra
  JZ 0)
   U B

B M XI
0) O w
Ni-l O
BXI lJ
                                                                                                                                                             01
                                                                                                                             O 0) .C
                                                                                                                             4J B O
                                                                                                                            I O O
                                                                                                                             M N  01
                                                                                                                          '    B  0)  01 V 0)
                                                                                                                             1-1  4J  4J 4J 4J
                                                                                                                              E  a  ra co qj
                                                                                                                              Cd rH rH T—I r-1 0)
                                                                                                                             r-l  CO  CO Cfl Cd 4J Ctf
                                                                                                                              C J5.fi JS J3 «r-l
                                                                                                                              ,!-< r-l XI O-
                                                                                                                          01  O  01  N X >,O<
      4J
   OJ 01
   B O
a)   E
                                                                                        d  H o)

                                                                                           Wrfi
                                                                                                                   (l)X)-rlr-m-l^( 0) 0) td

                                                                                                                   B  O  r-lnB  O  BXlr-IX! ,	_.
                                                                                                                   0)  1-lH  O  rJi-fr-l >,4JJJ4Jr-l
                                                                                                                                                                            (U
                                                                                                                                                                            c
                                                                                                                                                                            (U
   4J
   0)
   s
0)  O
                                                                                110

-------
                IA
                CM
        Si,
        i-i o>
        cd jj
        01 
                                                   OvO   OOOOOi-lO
                                                   oo
                                                   OO
                                                   ITl
              OOOOOO
              OCM
         rf
                ui
                CM
                         41 O

                         C
                              i-iOOO   OOOr--OO
                                         O            i-ii-i iA
                                    rt   co            OOO      •*
                                        >i-(Or>-OOOOOOOeMO
                                                                                                                         OOOOOO
        «M
        o
inmoo o
            JJ
       60    B

O JJ-H C O
^5  O ^™* ^ "^
•* ae i-j a.M


      SWI
                                                                       VD              CO
                                                                       i-i   i-it-i   CM
                                                                                                                     OO  .OO   O
                                       O'ao603B
                                       i-i js pen
                        B  E Oll-l
-------
 I
>
                 O U M
                 •U O ET
                    Cl-l
              o a» Ur-i
              10 JJ u 3
              CM co e a
                 ROS
                 3=0
                                               ^ vo co
                                          oo CM ONr~
                                  CO O    OO CMrH.
                                          o
                                          VO
                                                          o cyii-i
                                                          m CM I
   CM
o in

do
o
m
   •O    JJ
    8)13 C
    C 0! 0)
   §-^ OJ 3
   .n a i-<
-n  e a)
                                                                   a  «
                                                                  JJ  S>
              s
              a.
                                                           cu
                                                           a, e -o   .
                                                -   _  .   . .  Cu O CO  C  O
                   •i-t  cc ct) ?*•» !>%*^ i—(>COC}-jCO^J^OV-(CUC(}*f-1
                   S2HooofcjfcH<-<;cjcjuowjs:2:to
                                                                  112

-------
     CM
     f>
     O
     f-
     d
S   2
 a)
 3    S
 B    O
1-1    «:
 JJ    fa


 I    ^


*    ^
 !-<    O
 I    2
 >   M

 0)   Cu
      6M
      o
      ><

      I
                  i-l i-l    Jtl
                 > JJ  B  &. S
                 N  CO  03 »H cd
                  .-I  60^1-1
                   o  i-tH »
                  > o
                                                                                o oo
                                                                                odd
                                                           oo
                                                           do
                                                                 o oooo
                                                                 d dddd
                      C
                      o
                     i-l JJ
                      jj  is
                      3  ai
                     1-132
                      o
              irinOOOOOOO-*CMOi-i
                                                                                                     ooooooooo
                                                                                                     ddddddddd
                S
                Cb
                                                            m
                                                           "O
        •    o
      OrH OJ
     O   eg
         JJ  •
      a) o B
32 * MH E
 CL &, 3    <  -  -
      jj  -    1-1  as
 e  E cd a) a>  u«o
 3  3 Vj XI 13    i-l
 E  E <1) -r< -r4  . X-H j-l
2 S H O O  O !n
                                                            O
                                                           w
                                                      a>
                                                      CO
                                                      a)
                                                      01 to
 01
•a
 B

 O.
 to
 3  :
     B
     a>
     r-<
     <8
     >
     to
     X
                                                                        ,§
                                                                  a)
                                                                  03
   e
E  o
   (J
L
E 3)
O ~
                                              a>
                 C l-li
                 to 3
                                                                        e          «
                                                       m     0)          cs    M  M 43
                                                      •o     e       a) £    
                                                       u     N  a) 0) ra cu    u4Jr->0>
                                                      ^H     ojoicaajh    i-Hr-iC"-*
                                                      Si    £>  N £ 0) O    >i >»-r(  OJ
                                                       OOJOCUOi-l    43J3!>£
                                                                                                                                                         u js o o o
                                                                                  113

-------
     81  to
    r-l  O
    —4-H    J£
 O\ U  C O.C
 cr>  g)  s)t-i  a
 rHr-l  COUr-l
      O
o

d
oo

do
o

o
o

O
ui
eg
JJ
c e
o a)
•rl U 8
U O JJ
3 a) a
•-ise a)
o u
w H


^— 1

>i
<§


                           ooo
s
s
d.
                                                                                  0) 0)  C  0)
                                                                                  C C  to  C Q) 0)
                                                                                  t8 OJ3  0 C C
                                                                                 £43 4J £ 0) 0)
                                                                                  4-1 u  0) 4-1 i-J T-(
                                                                                  41 d)  E  0) •OT3
                                                                                  E e  o  E « to
                                                                                  O O  VJ  O 4-1 J-l
                                                                                  a M  o  E 3 c
                                                                                  O Of*  O A
                                                                                  u 1-1 m  M o
                                                                                 45 U-l i-l ,£)
                                                                                  O O -O ^H
                                                                                         O "O r-l
                                                                                                               n
                                                                                                            C i-l
                                                                                                      o  e  e to
                                                                                                      M  (0  tO r- >-< 
                                                                                                      I   0) J3 &.,£
                                                                                         14  l-l  1J
                                                                                         OJ  01 JS C
                                                                                         x: j: j->
                                                                                         OJ U  01 JSTI
                                                                                         0)  -. >^ o e o HD
                                                                                         C  C  M >M-I n-l *O
                                                                      114

-------
     (N
     CO
     o
•o
 CD

 B
 §
O
 d
      §'
                  0) ca
                  i-» O
                  •r4 1-1    ^i
               ON JJ C  D.G
               ON     3 o a)
               CM    I-H 33 0
                     O    H
                     CO    H
                8
                                                                                                                                 01
                                                                                                                                 u

                                                                                                                     X W §

                                                                                                                     °°S«2 3
                                                                                                                      t  I  3 r-H CO
                                                                                                                           OS 3
                                                                                                                                          o  o
                                                                                                                                          ajasa  i  cds5i-Hr-i
                                                                                                                                          4J  4J 43 al 6  -U  '   '
                                                                                                                                          a. a. a.u a 1-1 en ca
                                                                                      115

-------
      <*1
      f>
      O
      r».
      ff\

 o
f~4
43
      o
      Z
      £
     s
                01 IB
                   O
                u e  B.C
                (8 SJt-4 B
                   C    C
                   q    o
                  *•< u a
                  u a u
                   3 as a
                  r-IK 0)
                   o    u
                  to    Hi
 oooooo

 oooooo
            s

            3
            a.
            w
CMOOO VO c
PO
-------
o
o
     co i-l  C
     E  art
     O  Sr-l
     AJ  to pa
     3 co
                                                                                                  o

                                                                                                  d
                                                                 o

                                                                 o
                                                                  oo

                                                                  OO
                                                                     O

                                                                     o
                                                                                                                                                o

                                                                                                                                                d
      4-1  0) ^
      as -H  e
I-H    E  O. CO
O    O  Si-<
CM    4J  co to
      3 co
               CM

               >,
                                                                                                  o
                                                                                                  d
                                                                                                            o
                                                                                                            d
                                                                          oo
                                                                          do
                                                                             o

                                                                             d
                                                                                     o

                                                                                     d
    01 to
   T-4 O   J£
   .H i-l CuC
ON 4J C 1-1 CO
O  CO CO 1-1 i—I
i-l i-H W)H CO
    O W
   > o
                                                                                                    ooo

                                                                                                    odd
                                                                     oo

                                                                     do
                                                                       oo
                                                                       do
                                                                        ooooo

                                                                        odd do
                                                                                                                                                   o
                                                                                                                                                   d
 CM
 o
 co
         60
       1-1 C U
       0) i-l 01
     ft  O 0)
      COS
     CO O
                              in m
                              o o
                     O f-< m o O O O '
                                               Oi-lOOO
                                               -  -
                               i-t   CM    CM   oo    i-<
                    CM co CM CM o  in o o o   ~ ~
 O
 CO
      a
      Cu 0) kl
     •H  o a)
      U  t-l 4J
     fl  3 CO
      COS
      3 co
      T3    W
      Ol-O C
      e  o> oi
O    i-l  4J 3
O    &  CO I-H
to
                                      ^ -,.,-) 1-1
                                              o
                                             CO
                                           coal
                                           3D.
Mi— l-H
O4-'4J
   oe
                                                              Q>
                                                           O OJ
                                                           HCC
                                                            e e
                                                    CO         01
                                                    u    o)   •!-<
                                                    O    C    i-t
                                                    H    a)    1-1
                                                         £    "
                                                         4J  C -r(
                                                    co    .Ci-i e
                                                      jj a, 01 o
                                                              o>    o)                  e
                                                              •o    e       o)       CD  co
                                                              IH    ai       e       e 4:
                                                              M    Noiaica.    aicou
                                                              o    c c c x a) c jr  0)l-li-l
                                                                 o)  o^i o  o  --  -  -  -
                                                                      O t-lr-l
                                                                      •  o si
                                                                            o
                                                       o a)
                                                       CO C
                                                       u
                                                       U N
                                                    oj  oi e £ M
                                                    e  H 01 o o
                                                 01 i-l    Ji i-l i-l
                                                 e^a  e o 1-1 xi
                                                                                                                                               a> cu .c
                                                                                                                                               JJ 4J  01
                                                                                                                                               a) aii-i
OXE
oavita
paiffl
 OO
 vjVi
jsj:
                                                                 O-CTJ
                                                                 cxoci)
                                                                 oi-ia)
01
co       e s
01 X    33

Ss'ol'ci       S'oi^  5",3 fH  S-5 5. ClS'oi^H'U.rfHg yxl^
MOJi!a)<-IO-0>CcoeO>,NNXlOIC091  «OI r^OOCM^,
cjjoi-'coci-ii-iflixiaini-ieei-ii-KJ'X i t-i x icMcMr-itocnje
co aiiH  aixi-H  O-HJS o  cjcj u  4101 COJSCM OICMI-) g>i-i<-ii-i£riu
SS2COHC
-------
                    JJ dijrf
                    <3t-4  d
              o    e exes
              O    O Er-<
              .
      d
§J
    at o
   •-< O   J£
   *4*rl O.E
                 e «  „. .
                 -< eoHtn
                 5S
                        o
                        d
oo
do
o
d
o
d
      5
 u    K
I   S
§    s
   60
   B M
0)i-l 0)
 '  -t U
   O «
"    3
 ci    5,
              8   3
         U 09
      O  U 4J
         9 a
      c  o&
      SCO

                    OtJ B
                    B 0 01
                   Tt JJ 3
                      <8iH
                   .0
                    g
                   O blM
                   OHM
                                                                                                                                       CO CO CO CD O T* CO CO CO CO
                      to
                      B
             O
             CM
                      (X-
             g
             M
             S

             I
             CU
             W
                                                                                                                                                       B
                                                                                                                                                 .C  E -H
                                                                                                                                               r-l -rl l-l E
                                                                                                                                               O B  E «
                                                                                                                                               K CO  R) r-l r-l
                                   CMCMPMOCMf-i
                                                                              118

-------
               o
               o
      4-1  0) ^
      (Hi-IB
      E  Curt
      O  B 1-1
      jj  co w
      3 K>
                                        OOOOOl
                                                                                           > o

                                                                                           i o
o
CM
                      jj  o> .*!
                      « i-i e
                      E  O.S)
                      o  Ei-<
                      jj  to pa
                      3 w
                         OOOOOl
      CM
      CO
      o
    01 co
   1-10    X
   i-l iH B, B
O jj C-H  W
O CO   U
       i-l  O  01
        U  IJ  JJ
       1-1  3  a
        cos
        3 en
                                         o oo oo
                                                                                                                                                                         O O O OOO O
       *O     JJ

        B  01 01
 O    i-l  JJ 3
 O    JO  « i-l
 
-------
 a)
      Csl
      CO
      o
      !>.
      CO
      p:
      E
ID
F-t
 I
      M
      O
      >i
                  •a    ii
                   01 tJ e
                   coo
               Oi-( 4-1 g
               0.0 td.-l
               •»  B ojt-i
                   O kl >M
                  OHM
               00
                                                    lOOO
                                ITl
             ;    lAr-<    T-(    O m 1A      i—I
                 oo    o    ooo      o
           C»4OOOOOOOOOOOOOO

           ooooooooooooood
                     CJ)
                     C 0)
               rH    T< CO
               O    r-< C
                     o os
                     OH
CO

 >,
               CO CM
               oo
      ,-1 \o o-o o
                                   C>1VD COO Oi-H
                                           to
   )-i  01
oio-o
                                                            to
                                                           T3
   O
  ca

  •o
   0)
  •o

   o

38-
M  3  ^,
Q CO  B
                                                                          4-1

                                                                          0)
                                                                      t-l >
                                                                       td a
                                                                       4J X
                                          e  a
                                          DO
                                                                                01
                                                                               •a  oi
                                                                               T-l  B  0)
                                                                                14  BCD
                                   0)
                                   4J
                                   td
                                                                                   01  O
                                                                                   Or-l
                                 E  C i-l  B  B  d)
0)
to     SB
01     O  3
C r-l i-l t-(
td  01
                                                                                 : T3  M .M  0) —I O > B N J3 I
                    18 01
                    £ 4-1
                    4J Cd
                    J=r-(
                    Curt

         £  OO 01 P->4J
        JJi-4    B X J3 01
         01 js a oi oi a, e
    ~   H  O B rH JS
   to  01    1-4 0) td >»-< U
|J^-(  B  C  V4I-IJ3J3 >%td
0)  O  01  OH XJJ JJ JS
                                               01
                                               B
                                               01
                                                                                                       &
                                                                                                       4J
                                                                                                    OI 01
                                                                                                    B O
                                                                                                    01 1J
                                                                                                       o
                                                                                                                                          01
                                                                                                                                          B
                                                                                                                                          01
                                                                                                                           4J J3
                                                                                              B O
                                                                                              td td
                                                                                              B
   4J
   01
   s
o  o
Br-l
                                                                         120

-------
s
g
=   1
 I       VO
>   gs
 0)   MVO
S   *T
&   5
§
        in aj ffl 4J
             » «
           4)  DC
tM
sg-
        1-11-4  CJ=
        lA B  ffl 4J
        CMJt!  01 0)

        •  33°
           HI  DO
           CSV
          S^T! CD
          1-1  e c
                   f-i   uio      vo

                                                                  SenoooSoo o-o oooooooooo
                                         OVO^OOOOOO   r-IOOOOf»OOOOOO OOOOOOOO
                                         mCN«3-              ui                             v           y v
                                         r-tn                "•>
                                           O
                                                                                               , u-nn
                                                                                                 oo    oo
                                                                                                 OO    OO
                                                                                              OOOOOOOOO
        ...-CM
        O « « C
                               r-l CO   rH   00 rO
                               U
         s

         I
         CM
                                  a>
                                v a
                          K SC M «
                         .  OO.9 « ra 9
                                U U d) l-i
                           (3
                                        a
                                               to
                                               •o
                                             o o
            U O)

             U C
                                                            a
                                                        'r-l  >
                                                         (8  «
                                                  ffl CO >,
                           3 9
                           i I
                          •H «rl
                           (5 X
                         B B
fflOtJbrt  609C'OB99
V4    ^4J!^-l  I*W 0«H 9-H-H  1-1
-•  " H  B. B O    BBrffiSd)
                                                                                             0)
                                                                                             e o>
                                                                                     a
                                                                                     4J
                                                                                          fl)
                                                                                          C
                                                                                               l-l
                                                                                               O
                                                                                                          0)
                                                                                                          JJ
                                                                                                          eg
                                                                                                         i-l 01
                                                                                                          OJ 4J
                                                                                                         si «
                                                                                                          4J1-I

                                                                                                         •S.5
                                                                                 SB
                                                                                                41 OO 0)rH 4J
                                                                                                Nr-<   CXJ30)
                                                                                                c£ a) a) aj OH c
                                                                                                0) CJ
                                                                                                              0)
                                                                                                              s
                                                                                                              0)
O  .«  C O
                                                                                                            jBhaico
                                                                                                                  C
                                                                                    S'
                                                                                    ai
                                                                                    ai
                                                                                    o
                                                                                                                       tv o
                                                                                                            ffl JJ
                                                                               K 9 O
                                                                               JJ 1-4 Tl
                                                                121

-------
      ti
      g

^    I
ft    S
 I       VO
>    gg
 O
                0,0) U
                •H O Q)
             O O l-l AJ
                gco"
                                                                                                  i-<      ui
                                                                                §0
                                                                           ooooooooo

                                                                       'oo oo<
                                                                        V      V
                0) 00
                c c o
                -r4M (0
                   C O
             CN a O-H
                <0
                0)  60
                C  C
                *4*4 0)
             l-l r-l  B O
             o a  a c
             CM A!  OI-H
I
                                                                             m tn
                                                                        o   oo
                                                                             §00
                                                                           ooooooooo
             g
             M
             s

             a
                   ra
   CO
   •o

 Bf-i
 O O
j*m

 e-o
u o
   •o
 U B
•H d)
 B a
 a co !
                                                                 4J

                                                                 B
                                                                 0)
      0) CO
Bias P a
 a. a. 3 a) ra  3
     4J lj 0)  U
 sseo-oo-	
          1-1 J3 -r<  |J W
 BBO)U!Ua.CO    B.B*HBB
•Hf-ICl.   OtnO'i-liH.CVSOO
^ X Bi-i S  O B  u -• -•  "—  y •
-taa>rHi-HJ2Eo_ ^^(,«.
                                                                         .r-< u u js
                                                                                                            .
                                                                                                         W 4J.J!  B
                                                                                                              '
                                                                                                                         §
                                                                                                                         0)
                          0)

                          S
                       01  O


                       3  o
                                                               122

-------
 I
>
                   to
                   o
                   c ac
                                                                              o
                                                                              o
                                                                        oooo

                                                                        dodo
                    ooo
                    odd
                   01 60
                   e s 01
               CM. i-l T-I as
               OrH G C
               CM a) cd in
                      oai
                                                                                  vo
                                                                                  08
                                                               00    PI      O
                                                               1-1    O      O
                                                               ooooooo
                                                               ooooooo
                                                                                                   ooo

                                                                                                   odd
                   0) 60
                   6-B
                   •H IH  o)
                rH i-l E  M
                o a ce  c
                CMJli 0)1-1
OO 00 ON ON
                                                            O

                                                            d
                                                                     .o
                                                                     ooooo
                                                                     o o o o o
                    ooo
                      •   •  •
                    O OO
                                                              CO
                                                             •o
                                                           BrH
                                                           O O
                 -
                2
S3 S3
 B. d
                                      e
   01
a> n
IH cd    CO
3 01 to 3
4J IH 01. k   v
cdO "O O cd
 ea*o
U  0)
   •o

1H  01
 B  a
 cd  co  !
 MS  e'
                                        4J

                                        01

                                        cd
                                     rH >


                                     oa>
                                     HS
                                                                          E S
                                                                          3 S
01
B 0)
ed>o
                                                                                                                                01
                                                                                                                             .Ui-H
                                                                                                                             £ cd
 E E 01.
IH i-< a.
 B X B.
iH Cd O! '
S SHO
                                                 1-IJSiH IHW OiH 3iHiJ M
                                                  ^ D, C O    gfii-IEEOl
                                                  O CO
                                                  a o
                                                     g.*'
                                                           4J 4J 4J CO *D *J (H
                          I-H        01  O
                           Ot     01  OrH
                           JJ     C  IH £     B.J2
                           O     0)  O U  OlrH  4J
                          H     NrH     B  X4S


         CO     BE         o    0)  U
         01     33        co  0> X> i-<  0)
         BrH«rtiH     JnrHCOMrH.— .—  .
         CdOIBrH     OIOOIV,JJJUJ3

.	  60 Ji  01rHO>BNOlJ3
CuOCdBOrHCdBrHaJBrH-HiJ

"  '    ICS»(OIX!iHi-(.CO)43i-H01
       lESCOpsiOTKl       • ~
      01


      0)
     I-H



      JJ
   01  01
   B  O

-------
               eo
               o
               CM
                            CO
                                    CMOOOOCTVCOOI
                                                                                 •*       —I
                                                                                 OO VO    CM
                                          mr- r—vo I-H<
                                                CM
                                                                        CM
                                                                  CO    i-(
                                                                  moo

                                                                  odd
       CM
       o
 o    o
               o
               CM
                      60

                     •H  IH
                     •-1  0)
                      d  u
                      01  (8
                      E *
                                                                                 OO CO
                                                                                 rH CO
                                                                                  I OO O O
                                                CM          VO
                                                                  cOf-H (
                                                                  CM O <
                                                                                                     000
 CM    r-iOOOOOOi-IOOOOO
CO
tr\
O
               in
               o
               CM
C AJ
O B
•rH 0)
U U B
3 C OJ
I-H o> ca
OSS 0)
co IH
H


rH
CD
Q



CO
CO«3" OO OO
CM CO


CM
I-IOOOOOOOrHr-lOOC
CT\OOOOOOOOOOOC
voco


OO CO COr-H
OO r-HOOO
:>o mooo oo
3OOOOOOO


CM
o
~0
o


rH in ON in in I-H 1-1
O OCM OOO O
ooooooooo
ooooooooo
V V V V

 I
>
         §
         CM
                            cC
                            C  01
                           t-4 4J
                            C  CO
                            c
                                                                                                     VOf
                                                                                                     OO
                                                                                         ON
                                                                                         o
                                                                                                                            OO
                                                                                                                            --
                  m moo CM-*
                  O OO r-lO
                    i oooo
                                          CO CM
                                             VO
                                             CM
                        in co
                        VOCM
                                                                                                                                                   i OO
a    §
H    i-t
                                                                                            VO
                                                     oo                        vo in    vo o>
                                          OinOOvDoocrvoOOOOO- O O O O O
                                                                                              CM OO O OO
                                                                                              CM
o
d
ooooooooo
ddddddddd
              M
              g
        0-


        CO
                                         U
                                         o
                                             fl)
                                          01  to
                                   S3 S3  tJ  ei
                                                         CO
                                                        •a
                                                      B*-<
                                                      Or-l
                                                     .0  O
                                                      W CO
                                                      0)
                                                            OB
                                                         toi-l  01
                                                                             c
                                                                             01
                                                                             i-H
                                                                             CO
                                                                          i-H >
                                                                          <8 td
                                                                          e E
                                          01 t.8
                                                     T-IJSI-lCOOfH3lH'
                                                      M  O.O    B B tH B
                                                      OtO    1-HvHOIEO
                                                      01
                                                      ra     B  B
                                                      01     33
                                             h  .      B rHlH tH
                                             01        td  01  C rH
                                             D. E T3  OOJii  0) rH
                                             a, o  «  B  O      '
                                                                                  124

-------
                  a> co
                     O
                           .
                .u B  O,E
               ON CO CO «H CO
                                                                                                     oo
                                                                                                     ooo
                                                                                                     ooo
                                                                                                        O

                                                                                                        O
                                                                                                                             O
                                                                                                                          ooo
                                                                                                                                         o
•a
 o>
 s
I
    t     C B
    ODrH  O 0)
i-l  O  «  o 3
Oi-J  O  bOi-i
            w
                                                                                   VOCM    f>   ff*   I-H    in             •<* 1-1
                                                                             o   oo    o   o   o    o             oo
                                                                      >t-iOrr>OOOOOOOOOOOOOOOOO
                                       O-vOCM-d-
 I
>
       00   ±1
       B    C
      •H  e a
O    i-H i-l 3
O     4J  tOt-l
-3-     4J  OHM
       0) CBM-t
      tn    ta
                                                                                                       >oo
                                                                                                   O
                                                                                                   O
                    rH    r-l          i-l-*«N)
                    O    O          OOO
                    ooooooooo
                                                                                                                        ooooooooo
                O   t-i E S
                >-l   >rl Sl-4
                CO   O-r4*M
                         COW
                  >,
                  s
                        -*OOO

                        in wJoor^Ato
                                                                              rIOOQOCM
                                                                                                   com
                                                                                                   esjO
                                                                                             oo    m m CM m <-i »-i (o <»•) r-i i~- I-H
                                                                                             r-i    OO O O OO r-l i-HO O O
                                                                                                 ,00000000000
                     ooooooooo
                        V  V  V *V  V
                     »o
                      0)
                      e
                o
                CM
                         S-.4J
                            CO
                      003=
                                                   <£>
                                       co oooooooo
                                              CMO
                                          CM CT>
                                          CO
                                                                                                  •ooooooooooo
                                                                                                            v v v v v
                2
                               O
                              O
                                  CD
                               0) CO
                         as w tJ «
                                                             CO
                                                             •O
                                                          B i-l
                                                          O rH
                                                         •JO
                                                          H W
                                             -a
                                           CJ  C
                                        «>•<-!  a)
                                                                         <0 <8
                                                                         -U X
                                                                         o 'tu
                                                                         H 33
                                                                         0)
                                                                         co
                                                                         0)
                                                           i    i B-r4 E e 0
                                                             r-li-1 0) E O O O.B-0
                                                                                        B 0
                        <   0)
          0)                4J
          B           O)    CO
          CO          "O    i-l
         f 0)       -r(    CO
          U B        )-t    43
i-l        0) CO
 CO     0>  O J3
 4J     B  I-l U     4NO>CD 6 N O  »  CO O
                                                                                                                            01
                                                                                                                            B
                                                                                                                            ai
                                                                                                                           r-l
   4J


B§
0,^
   0)
   01


  !
   0)
   o
at o
                                                                             125

-------
         CO
         o
         CM
                           to

                           •rl U
                           i-H 01
                           cd jj

                           15
                                   "1 t^ CM CM rH r-l
                                         CM
                                                                                                                              CM

                                                                                                                        o    8
                                                                                                                        o    d
         fs*
         o
         CM
Annealing
Water
CM
Sh
m
Q
                                   u")VDuiOOOCMr>OOOOOOOO
                                         CM            v
                                                                                         00

                                                                                         do
                                                                                                    VO    O
                                                                                                    ooo
                                                                                                    ooo
                                                                                                                        o

                                                                                                                        O    O
         CM
                        B   JJ
                        o   e
                       T-l   0)
                       jj jj a
                        3 03 JJ
                       r-l 01 «
                        OK 01
                       CO   M
                             H
                                  I
                                                                                                                        Ot/1    r-l OM3S i-H rl rl
                                                                                                                        OO    Oi-li-IOOO
                                                                                                                        ooooooooo
      CO
      "O
      o
                  c
                  o
                  3 C JJ
                  <-i 
 O
r-l    <
J3    CO

5    fe
     »


     %
CO
            •o to    u
            01 O    C
                        0)
                        CO
            jajd c  a  c
         tM H O OJ.iS.rf
                  ei  to
        CM
        o
        CM
                       r-4 c  en
                       a a  a
                                  CM

                                  s1
                                                                                                          OO   rHi-H
                                                                                                          ooo
                                                                                        rii-toooooooo
      CM    rH         t-4    ITl
      o    o         o    o
      ooooooooo
                                        OOOOOr-»tJ»OOOOOOOir>r-iO
                                                                                                   ooo
                                                                                  VO
                                                                                  rH t-H
                                  CMvOeovOOO-*OOO
                                        CM
                                                                 OOCMOO   O O
                                                                                                         CM

                                                                                                    00 OO OOO

                                                                                                    CMOO odd
o    ooooooooo
d.ddddddddd
        g

                                                 d)
                                              0)  co
                                                 O
                                                            CO
                                                           •o
                                                         C«rf
                                                         O<-(
                                                         J2 o
                                                         VJ CO
                                                         ctj
                                                         U>O
                                                           'O
                                                         o C
                                                       >i-< ,
                                        3
                                        E
                                                                     4J
                                                                     e
                                                                     <1)
                                                                    r-l
                                                                     si
                                                                 r-l  >
                                                                  cd  CQ
                                                                  4J  X
                                                                  O  OJ
                                                                 H 33
                                                                  BE
                                                 0,0
                                              OB
                                                            ei-i  E  s S
                                                                                      3 S
                                                                                     •rl 0)    33
                                                                                      CO C fl*rl •<-!

                                                                                 ! TJ  B bO^ 0) r-l
                                                                                                            Ol
                                                                                                            B
                                                                                                            cd
                                                                                                            f 0)
                                                                                                            •U B
                                                                                                            ai co
                                                                                                          a) ox;

                                                                                                          a) o a)
      o
      i-i
   o) .e
   eo
                                                                                                                                   0)
                                                                                                                                   u.
                                                                                                                                   ct)
                                                                                                                                   i-l C)
                                                                                                                                   cd u
                                                                                                                                   X! cd
                       0)
                       g
                                                                                                                             rH JJ
                                                                                                                              KX! 0)
  JJ
0)  O>
c  o
01  IH
                                                                                                                                   01 j3rH
                                                                                                                                   U JJ.B
                                                                                                                                  >
-------
          .  0) a
           rH O   AS
           •*•** C.B
        ON u BI-I  w
        ON  « at prH
                                                                                             in         00
                                                                                             CMrH       O
                                                                                             00       O
                                                                                             ooooo
                                                                                                  O
                                                                                               oo
                                                                               ooooo
                                                                                  V
                                                                                               oo
                                                                                                                                              O
                                                                                                                                           ooo
                                                                                                                                           ooo
                                                                                                                                              V
CO
in
o
              03
              &.Q)
                 3 «
                         CM
                                                         in      oo         tn
                                 CM ON                   O<-l   i-l    ON   O
                      Omo    r-CMinOO OOOOO«» OOOi-HOO

                      in in CM    OOO^OOOOOOOCMOOOO'OO
                                                                                                                     O       O
                                                                                                          O       OOOOOOOOO
                                                                                                     O      OOOOOOOOO
•o
 8   i
.5   e
*».
I   3
3
oo   o

7   S
>  .g
 jj   S*
f—I   2
.o   co

*   is
                    4J
            i    e a
            60r-l O O
            O « O 3
              O 60»-l
              If
                                                                               O    rHrHVI
                                                                                                  f-H    IT)
                                                                                                  O    O
                                                                                                oooo
                                                                                                                                in    i—I rH rH P*»
                                                                                                                                O    OOOO
                                                                                                                                O    OOOOO
                              m m r^ CM o o !••• CM o o o o o o o o o o o o o o o o o o   oooo
                                    •_< ^
                                       CM
                                         vooo
                                                                          OOIAOO   r-i i
                                                                                               (•         CM

                                                                                               >oo   o

                                    in <0 os? ddvoooddddddddddcnddddd   d
                                                                                                           o   o
                                                                                                           ooo
                                                                                                           ooo
                                                                                                                 V
                                                                                                                           o
                                                                                                                           o
                                                                                                                                 OOOOO
                                                                                                                              t»i\o CM
                                                                                                                              000
                                                                                                                        ooooo

                                                                                                                        odooo
o
rH
CO
eou
B B
!§
S3
CM
...4
CM CM OO.BO
en
S'oo
OOOO
OOOO
V V
                                                                                                                                 in ir> i-t CM »-<
                                                                                                                                    §0000
                                                                                                                                    OOOO

                                                                                                                           o    oodcJd
              •o
               0)
               6
                                                                                          >n
                                                                                          o       ooo
                                                                                 >OOOO    OOOO
                                                                                                                                 i-i   m«n   ...
                                                                                                                                 o   oo   oo
                                                                                                                                 o   ooooo
                                                                                                                                 ooooo
                                                                                                                                 V V    V
         g
                               33 S!
                                                        CO            4J
                                                       •O            B
                                                     C-H            a)
                                                     OrH            rH
                                                    JO  O            3f'
                                                     VI CO         rH >

                                         6~         O -O         4J X

                                                     OB         H S3
                                                  eo-rf  0)
                                                to 3 B   «
                                          -   .   6) l-i «  m  >,      E S
                                          BJO-O O 60J3  B O B 3 3

                                                  g.-rt  "  a,--5«'S
                                        0)
                                     t-i
                                     Q> «» (-1
                                                                S a)
                                                                   01
                                                                   to
                                                                   01
                                                                   B.rH.
                                                                   03 
                                                                                                   •u B
                                                                                                   a> 03
                                                                                                 01 O.C
                                                                                                 B W t>
                                                                                                 0) O 01
                                                                                                 NrH O
                                                                                                            0)
                                                                                                           •o
                                                                                                         0)  0) 01 0)
                                                                                                         4J 4J 4J 4J
                                                                                                         CD  cs a t-lr-l
                                                                                                      O 0)    CX
                                                                                                      '
                                                                                                                 iJ 4J  4J
0) U
4J CD


.3
_C ij
tijS
                                          oca   f-(i-((l)EOO&.C'O eo^  O !> C
                               fl 03 0>
                                                O  O B
                                                                                   «-i 41
                                                                                                 _^MPPNO)OIO)N..
                                                                                                 Q)  O O O 4-1 B B rH  «-*, B W 4J
                                                                                              CDja>r. ID 3 U

                                                                                              S) MH O I-l i-l rH >,4J  JJrH t  t
                                                                                              N O  I « p Q >>4S J3 W XZ Z
                                                                                              B rH rH
                                                                                                                            UOJJ5
                                                                                                                            0)
   0>    01
  rH    B
   >»  ' 01

  •£    rt
0>  0)    UM
BO    U
01  h    01

   0    S
     a) o
     B rH

B* S 3 O
                                                                         127

-------
         CO
         o
         CM
                      60
                      E
                      Oi  cd
                              CO
                                                                               \o
                                                                               CO l-H    rH
                                                                                >|-
rH 01 a
   !SB u
      M
      H
                  co"
                                                                                                   CO CO
                                                               oo         tn
                                                          mo         co    oO   I-H
                                                        4rHr-4OOOOOOOOOO
                                                                               CO
                                                                               O
                                                                               o
                                                                                                                             t— I IO OO r-l r-l i-lt-l    i-l
                                                                                                                             OOrtOOOO    O
                                                                                                                             ooooooooo
§   5
B   «
s   S
eo    p
f™*    55
 •    3
^    »J
cS
                     60
                     B 01
                     B ra
                     B CO
                             CO
                                                                        COCO
                                                                                          CO
                                                                                       cots
                                                          h»    <*       CM   co
                                                          VD    O       O   O   OOO    OOO
                                                          oooooooooooooooo
            •O 60
            61 B
         O.O.M c ffi C
         CM s o
                                         CM         CMCM
                                                                                                                            o
                                                                                                                          OOOOO
                                                                                                                          OOOOO
S
         s
         CM
                        eu  to

                       •H-rl  01
                       r-l  B  CD
                        a  a  B
                                   r*» o\ so t**. o o *
                                        copg
                                                                                                  oooooo
                                                                                                        V V
                                                                              o
                                                                              d
                                                                                          i-l         CM    CM
                                                                                          o         oo
                                                                                    ooooooooo
                                                                                                                            ooooooooo
         o
         0»
                           E°
                          •r*  0)
                          r-4  CO
                          ^  B
                           OM
                    PM
                             CO
                                              VOCM
                                                                CM
                                                                l-H
                                                          i-
                                                                                       oi  o  01
                                                                                                                       0)
                                                                                                                      •o
                                                                                                                    0) J3
                                                                                                                                   01
                                                                                                                                  4J
                                                                                                                                   a
                                                                                                                                  1-1 «l
                                                                                                                                   a u
                                                                                                                                  js a
                                                                                                                                  4J r-<
                                                                                                                                  £ a
                                                                                                                                   O..C
                                                                                                                    C CJ  01 r-l 4J
                                                                                                         Ni-HOBO)    BXJ3
                                               00    rH^tO)BOOO.B«O 60^! 0) rH O  >  B
                                                     BB        "OIOOOBBrH.fi
                                                     33       COO),Oi-lrHtMa>a)a XrH
                                                      '«-!.   iHrH B O  (H ^j .O.iO i-H J3 .jc N
                                                  <1)  B rH    0) Q 0> H H  O IH rH >> 4J U-J3-
                                                                                                              a o
                                                                                                                                              0)
                                                                                                                                              B
                                                                                                                                              01
                                                                                                                            OJ
                                                                                                                            O
                                                                                                                            IH
                                                                                                                          0) O
                                                                                                                          BrH
                                                                                                                                0)4JO>4Jr-lT4
                                                                                                                    01  0)
                                                                                                                    B  O
                                                                                                                 0)  d>  rl

                                                                                                                 0) jCrH
                                                                                                                 U Uf
                                                                                                                  "  B  CJ
                                                                                                                    a  a
                                                                            128

-------

"•>
P
                 0) tO
                 i-H O    .M
                 «rfi-l  O.C
              o\ u e i-t  eg
              ON eg «  V    VO
                                                                                 eg   o    OOOeM
                                                                                      §O    OOP
                                                                                   oooPOO
                                                     ooooooooo   ooooooo
                 ro
                 o
              ooo

              odd
•o
 o>
 3
 c
1-1
 4J

I
J2
 a
H
g


I
o,
      o
      >*
         e  a
         o  fl)
      «8 O  3
      U BOi-H
•Sf Ol-< BJM-I
•H O
                                                          oo       •*         u->
                                    os                    o\r>-    os         o
                      omooooo-ooooppppppppopp
                    60    4J
                    C    C
                    i-l C  0)
                          S
              O    -IM S
              o    jj m<-i
      CO   Ed
                       e a
                       i-l 0)
                       E 3
                               f
                                       in ev)
                                       CM I-H
   o   oo
oooop

ddddd
   V    V V
                                                                                                    OOOOP

                                                                                                    ddddd
                                                  O      vD i-H i-l CM   V5    CM O         O   OOOO
                                                  — — —   •-"    — — — — — - — —  ~ — — — — -~> Q t^i
                      iri mo ©OOOsn. OOO OOO-*W<-< OOOOOOO OOO OOOO<
                                                                                                                     OP
                    •o
                     V
                     e    o>
                    i-l >,4J
                    .D<-< CO
                     Bi^ «
                     oo*
                                                                              ^ r-i   \Or-ICM    i-l U1 i-H    i-l i-l i-(    r
                                                                              CMO   OOO    OOO    i-li-lp    t
                                                                              —poo oooooo OOPO<
               2





r_j
o
V to
,sd as >-i a
09
•0
C T(
X) O
U CO
eg
o-o
•o
t) B
OJi-l 0
jj
B
0
ea
!-< >

•u X
•&£

                                           JJ  !-> 0 >j eg  co
                                             >.»
                                                                    e  e








0
to
0


,


f_l
eg
o
H
•i
to
0
B
eg
.c
jj
0
0 O
B V4
0 O
Nl-H
CX!
0 O



0
B
CD
f
0
2
o








I-l
o
0 J3i-l i-l >W







0
0
N
B
0

0
•o

^4
O
r-l
6
0
B
0







jj
eO
l-H 0
eg w
ij2 Qj
JJ r~4
x: eg
o-x;
0i-< jj
B
0
f-H
eg
xx:
0 CU
XI
>srt







.0
B
0 0
B U
0,B
0
C
0

^^
x;
jj
0
o
M
o
rH
0 JJ.C


0
B
0
r-l
>>
JJ
0
O
M
0 O
                                                 O co
                                                       >     a BI-I s  a  0
                                                        i-ii-i 0 e o  o  B-B-O
                                                                                        CJ > B  N  O  I

                                                                                       •i-l ^ XI  0 XI i-i
                                                                                                                                 0) Oh
                                                                             129

-------
         to
      •O B
      O-r<  01
<-4    Ur-l tJ
IT)    a.*!  to
•*    o) o  a
                                                          00
vovoo
                       r^ooo
                            CM
                                     o-*o

                                     indd
                                               oooo
                                                               §00
                                                             Of-H
                                                               oooo    ooooo
                       r-.COO
                                                         VO                   IT)
                                      rH                 CO      VO f».     i-IO
                                   oo-o    o©oooo"">coocMr-.\oo

                                   ooo    -4-o o o d d VO-CM ddi^^d
                                              co              co
                                              CO
                                                                       XJ
                                                               CM ID   O   OO
                                               OOOOOOcOi-IOOOvOI
                       VOOOOOOi-4OO
                            CM      rH
                                                                                    CO    t-l
                                                                                          §o
                                                                                       oooo
                                                                                    ooooo
                                                                                                    00

                                                                                                    c5o
                                                                                                                                      o
                                                                                                                                      o
                                                                                                                                oooo

                                                                                                                                dodo
O
O    «Jr-l

      w
S
CO
                                O
                               1-1

                               €

                                o
                                    a)
                        to
                       •o
                       >r4
                     Bi-l
                     o  o
                    Xl CO
                                          O 0)
                                             •o
                              .  ..  .      OB
                              4  @ Q    09 *H O)
                               < 0) a  3 B CX
                                                            4J
                                                            a
                                                            ai
                                                         10 O
                                                            X
                                                            fl)
                                                                                                       0)
                                                                                                      •o
                            B Q) 0)  0} Q)
                           •r) 4J 4J  4J 4J
                            B to «  « to    ai
                            tO i—I r-l i-l i-l 0)  4J
                           p1^ Cd (0  Q) Cd XJ  CO
                                                                                                           01 4J 4J 4J JJi-l  CO
                             ,ee
                                       '
                                        0.0
                                     oo
                                                   «rl 3-rt.rl
                                                    c 1-1 s  e
                                                01

                                                01

                                                US ai
        4J C    01    Wl
1-4       01 «    p    o
 «    01  OJ=   A   r-(
u    Bku    oaix;     aa.&,
 O    OIOOI   4JBUOIMr-4<-l
H    N i-i o s  o  :     .:_::;	_
      BXIWPI-lNOIOJOOINX ^,CL(

 00 01 Xl iH i-j 'Wi-IOIOlCOOxSs'Ot-t
i-H-B' O U iC 6.,ej^!»j-e  u -  - ^ -  •
 O Q) tj H
Oi

V
                                                                                                                                         B
                                                                                                                                         0)
     4J
     01
     o
                                                                                                                                  jJ2010
   0) 01
   B O
0)  Q) h
B  M O
                                                                  130

-------
       00
       O
       CM
                       •O  60
                       01  e 01
                       C i-l U
                       fl r-1 B>
                       ,fl ^ OJ
                       II  OS
                       «>•*
                       OS*
f> MO
    •  •
    1-3-
     CM
            OO O
                                               in in
                                                 §O
                                            CM OOO
                                            r-l v v -3-,
                                                                      O
                                                            oooooo
                                                            COOOOOOO   i-iOOOO      r-t
                                                                                      VOVO
                                                                              in«3-   I-ICM
                                       \O»DCOOOCOOOOOtnOOOOOOOOOO
                                               v v tn
             60    B
          *O B U  Id
       vov-ifi B  o
       O  O i-l 0>i-l
       CM Oi-l O.t-1
                                  I
                                               o
                                       o oo o
in an\o o o-*
     I-l V V »-4
             o
     •o
     I
      §
     o
          s
  o
Wfi
zo
HI ON
     2    sT
      I
     >
             3c?v,
        m    o~* w
        o    o i-< u
        CM    U O td
                        4J
s
           3
                  co
                  O
                  CM
                   o
                   CM
                        o o  a
                        BOS
              4J
              o
              td  M)
              JJ  C M
              B«-< a)
              O rH U
              O  O ft
              e  o,S
                                     in in
                                       o
S
                                        o-o
                                        CM m
                     oooooooooooo

                     vor^OOOOOOOOOO
                        in
                        CM
                                                                                                       ?
                                                                                       CM   OO   OO                 O              OOO
                                                                                       oooooooooooooooooooooooo
                                                     -3-CM-SfOOOOOOOCM OOOCM
                    0)
                  I 4J
              0)i-l  «0
         _    B o  id
         o    i-i ess
         CM    .fl
              8 u  6t
              O O  B
              OSS i-l
                                        OCOO
                                             i-i      m
                                                             OCMOOOOOCMi-lOOO
                    2
                    a
                                                                                                         O O AJ B Si-l
                                                                                                                01 01  «
                                                                                                 B o m= o
                                                                                              O  Ol M EH  CJ M i-l T-l &s 4J 4J
                                                                                                 N o>  « 00
                                                                                                         X^-i
                                                                                      131

-------
                       to
                   •o  c
                    0>-r)  01
                   4Ji-< 4J
                    &#  2
v^    SO
_     M°>
*    .Jr-l

S    I
       CO
4J     *.
43     O
S     X
                   U 60
                   01 B  1
            S
                0)  tn
              -r-l  O    Ai
            P>ir
                                                                          e  s
                                         O.C  c
                                                           P CO  O-H
                                                        U.O     B  S-
                                                        m    1-4 >r(  a>
                                                                       0)
                                                                       CO
                                                                       0).
                                                                                                          CO
                                                                                                          JJ

                                                                                                          t5
    01
    c
    CO
   jr at
    •U B
    01 CO
:41 O J3
 B h 4J
 01 O 01
 Ni-l O
 B J3
                                                           S  01
                                                           p  a. B-O
                                                                                                    01
   O  0) JS
   U  BO
Spa)     B «o
 B  a)  «  at  oi
•rj u  aj  u aj
    CO  CO  ca  s)    o>
   r-11—i t-, >,£
                                                                                                                      OOJJfiErHCOJ3CJ'JJ4J    »H
   01

   01

   >,
  42
   JJ
01  01
B  O
0)  14
lj
                                                                                                                                                                  01
                                                                                                          4-1

                                                                                                          01
                                                                                                          O

                                                                             132

-------
            00
            O
            CM
                  •a      ;
                  Q)    Q)
                  C  >>4J
                  O
                  O
                              CM
                             jco
                             •  *
                            00
          CM
          CM      CM L   ,
OOOOOOO«*CMvOeMOOI--O

   CSOOOOCMCMrHOvOOOrHO
                                      R
4J
60 e
•o c ,u «
OSrHo
                                       OOOOv
                                        •  •  *  •

                                       r-4 V v \O

                                                                         \O CT* ONf^
                                                       i-l CM
                                                         •*
JJ
60 e
vO ^>t *»"t C t)
O OrH «rt  «
OrH  4J
OOO)

&.S*
                                  ^•oo
                                    •  •  »
                                  vO r«-oo
                                                OrHfHinOOOO
                                                                          ONON    i-i
                                                                     OOOrOOO
                                        oo      I-H              m
                                   O\   rH      O
                                   CMOOOOOOOOOO
                                                                                                                                    m        t-n-H
                                                                                                                              o    o        oo
                                                                                                                                    	ooooo
                      I  0}
                   •OrH  U
                   a)i-i  m
             o    c o  at
             O    t-l OS  5=
             CM    .O
                   ^ U  61^
                   o o  c
                   CJBJ-rl
                r«(OO,

                VO I-.I-H
                             coOOONOOOOOOcOrHOOO      i-*
                           M
                           o
        a)
        4J
      01 O

ILIt^
     o o
     JD CO
     tH
     cd-o
     O 0)
       •D
     o c
   C0*rl 0)
09  3 e cu
                                                                     rH >
                                                                     ss
4J
O
P+
                       e
                       C)
                       j-0)
                       UC
                       s,iJ4JUrH
                                                                                .
                                                                                JS 4J
                                                                                JJ .C
                                                                                J5 & ffl

                                                                                fl<    e
                                                                              AJ
                                                                              0i-H^O
                                                                              O >, J3- «
                                                                                                                               d) 0)
                                                                                                                               CO
                                                                                                                               0) Jj
                                                                                                                                 o
                                                                                                                              iJj3

                                                                                                                              C 0
                                                                                                                                                         fl)
                                                                                                                                                         e
                                                                                                                                                         (1)
                                                                                                                                                         0)
                                                                                                                                                         p
                                                                                                                                                         rl
                                                                                                                                                       6)0
                                                                                                                                                       0'-*
                                                                              133

-------
           to
           B
  ON
  in
  CM
                                                                       VO
                                                                       1^-   CO

                                                                    OOOCM
                                                CM         ON
                                          OO-3- i-)OOO
                                                                    OOOO
                                                                                  O mO r—OOO
                                                                                  O ON   -tfO m
                                                                                  o         «d-f-t
                                                                                  O         i-l
                                                                                  CM
 CO
 m
 CM
           CO
                          .M B
                           o«
                          PM
                  CO
                                                                  OOmOOOO
                                                                    OOOrH
                                                                                       O •* O in O
                                                                 co
                                                                 CM
          to
       •O B
        S.1S CO
        ai o B
       >l~4 9
       H&.
                                        co
                                      i-ICMO
                                                                                    CO    CO
                                                                 	             CO ON    CMCOf-
                                                                 ooooooi-tooococoo
                                        VOVOCM
                                             CM
                                     vooo
      **

      a

X   §
I    e

1    rs
s    s
 O      ON
O    CJJ-H
>-"   SO
_    WON
O*    i-3»-4
l-t    B<
^    5
1    °
S    X
                       sue
                 O    3 0) 8)
                 O    3 U g
                 CO    Uf-4f<
            bl
                       lj CO
                       0) B

                 •*    l-<«rl 0)

                 CM    > O B
                       4» OS
VDONO


VOVOCO
                                                ooooooomcMmovoo
                                     vooo
                                        **>                       i-( •* VO fO CM 1-4 O
                                     Ol-IO   OOOOOOfOr-lrHOOVOO
                       VDOM-4
         T4 a
    a  si  LJ f-i
   t-<  BOH pa
                 CO
                                                                                                       O    O
                                                                                                       ooooo    oo
                                                                                                       ooo oo    o o
                                                                                                                          IOOOOOOOO
                                                                                                                     m
                                                                                                                     f~.
                                                                                                                     o

                                                                                                                  ooo
                                                                                                                   •  •  •
                                                                                                                  ooo
O    U
O     Wr-l O
•a-
                                                                                                             m m tn m           in m
                                                                                                             0^-100           o o
                                                                                                                     o   o    oooooo
                ^     0)    M
                O     VQ 41
                CM     M B U
                i-<     3 O B
      CO
                       COVOO
                                                                                                                oooooooooooo
E
I







tea
CUD





Or-l
o B
U
4) O

'i> «
O
s

o


. 0)
B B (
< 4) co :
Jj 41 1
CO
3
o o
J2 CO
(-1
B-O
U 0)
•O
U B
a i-l o>
3 C D,
J B CO









(^
                                                              4J


                                                              4)
                                                           rH >
                                                                                                                                              tt)
                                                                                                                                   B  B  B) « AJ B
                                                                                                                                   C.C.C.C Bi-l
                                                                                                                                0) 4J OJ 4J U<-H B
                                                                                                                                J3 J3 J3 J3X! B.B
                                                                                                                                G, D, Dj

                                                                                                                                -rHi-lf-4       JJ -fi
                                                                                                                                              .C!(l<
                       OSCO
     UTS -O    ^43  h CO
                   o> O iJ J3
                                                                                                                                t-l J2 J3 J3 O Xj:  B B U
                                                                                                                                4JU1-II  IXiOJ^lBB
                                                                                                                                                 41 J3 B tj
                                       3
                                       B
                                                                 134

-------
             OO
             o
             CM
         60  |

      011-1 a)
      Bi-4 i-i
     i-l Jrf 10
     42  o a


     o
                CM CO CO
                     CM
                                                  u^ o O
                                                                         CM                          !"••
                                                                         r—      \OI-ICMVO         O
                                                                o oooooi-» cou">*o oovo p

                                                                                   4 O O ON O O CM O
                    01     0)
              er*    fi  >»JJ
              O   f) i-<  CO
              CM   4ii-l  ttf
                    o
                    u
                                             U1U1
                                               SO
                                                     i-l            VO
                                                     ,_<   ,-too r—"">
                                       ^ o o o o o   I*** cj\ o o T—4

                                       OOiAOOOO   COOOOO
                                                                                          i-IO
                                                                                     r--oooo
                                                                               vo co      1-4
                                                           «-4 OO
                                                                                           CO
                                                                                     CO    r-4
                                                                                     t-iOO

                                                                                     odd
                                                                                                                          o
                                                                                                                          d
            JJ
      60    B
   •O B JJ «d
\O 1-4 «rl B O
O  Oi-l Ol-r4
CM 01-1 a- t-i
      O 0343
      e!    3
                                             U1U1
                                             OO
                                     ui MS O O O i~»
                                          CM V V ON
                                                           OOOOOOOOOOCMOO

                                                           ooindddddddi-iod
•o
 0)

 B
I
              01
              O
              CM
a 60
JJ C M
Bi-l 0)
Oi-l JJ
o o a
                 CO
                         mm
                         OO
                                        O>
                                                                  i-lOO   O
                                              iriOOOOOOOr^OOO
                       vo o OOOOO    \0«3-OOOOOOOOOO
                             f-4 V  V          f-4 O*
                                                 co
                                                                                  V    V V    V
 t
>
              CO
              O
              CM
Noncontact
Cooling
Water
CO
I
                                   §o   in
                                   O Oi-i
                                                                                                                                                            §00    o
                                                                                                                                                            oooo
               o
               CM
       8 60
       JJ B  M
       Bi-(  0)
       Oi-4  JJ
       o o  cd
       B OS:
       00
               O
               O
               CM
                        t  6)
       01i-4 05

       •5,2:1

       E JJ 61
       o o sf
       033 i-4
                                                                                                          CO      i-l^-l
                                                                                                                                   in    iri    1-1
                                                                                                                                                          mtn ^H   i-i
                                                                                                    CMO      OO            OOO         OOOO
                                                                                                    r*. OOOOOO OOOOO OOOOO OOOO OOO
                                                                                                               v    v    v
                                                                                                                                      v  v  v    v
                1-1
                2

                3
 O

£
                              01 O B
                        sdsa MH a
                         O. O. 3    •<
                                                                CO
                                                               *O
                                         O O
                                         43 CO
                                         nCO
                                         O 0)
                           4J   .  01         *O
                           -  -  co       OB
                                 (d    co 1-1 01
                                 0)  to 3 B Cu
                        _        p  a) M a to ^,
                     EtdO)0)U'OO603B
                                                                              s
                                                                              0)
                                                                              <-<
                                                                              cd
                                                                             l >
                                                              BE
                                                              3S'
                                      .
                        Si-li-li«  fc O-O
                                          ^
                                                        B-rf6EQ)
                        i      0)
                        S ;S H 000 Pu
                                                       --1X!
                                                       PuEu
                                                                                                          1-4
                                                                                                           a
   01
   s
   a
  43  01
   JJ  B
   oi  a

S25
01 O  01
Ni-4  O  B O
        C
        •O
                                                                                                                         B 0)  0)  0) 0)
                                                                                                                        i-l U  U U U
                                                                                                                         S OJ  O  03 05
                                                                                                                                          0)
                                                                                                                                       cu 4->
                                                                                                                         1-1 a  a  a  a JJ «
                                                                                                                         e 43 4=4:4: oti-4
                                                                                                                         a) jj  jj  jj
                                                                                                                            S  ef-
                                                                                                                               01
                                                                                                                                       O. D. CX
                                                                                                                                                     43 JJ
                                                                                                                                            01

                                                                                                                                            0)
                                                                                                                                    B "0 X
                                                                                          M"BO
                                                                                                   01  U O O JJ B
                                                             HH«OOOOl-l
                                                                      Ofijif 01 i-l O  .   .
                                                                      B  U r-l Cd B 1-4  01
                                                                      cd i-4 01 43 *H i-l 43
                                                                     S Z CO H t^ CO PJ
                                                             _  -  HJ3
                                                       01  O  01  MH CJ
                                                       >  B- N'  Q; '  «
                                       I
                                     0)  0)
                                     B  O
                                  ID  AJ"   r-l 0) 43 r-l
         0)<8O>ta)3Oi-4>-.UJJ43
O C fO r^ iF- ^ J-* ^2 «O  O  ^>.C (d C  O
ij 1-1 r-<  >-,jj jjjji-ii-  t43xjps43 43 si P? '^Iz ? •" S ^ *?  H
r-l I 43  JJ  CuZ  tjjt  t  01E4J01JJ
         -•     'CM3^-ii^i^Tit;43.ai
   01

   0)



  I
   0)
   o
   M
01  O

0)43
                                                                                  135

-------
               •o
               01    -,JJ
         O    «!-( 0
         «*>    «-r( B
               U03:
                                                                            CM
                                                                            o\
                                                                            oo
            JJ B •!-! O
          l « B UHI
            rH COHCQ
         O
         O
              •O
               a)
               «!-(  tO
               «»•<  B
VD
m
o
CM
                  68
                 i-4 a
                 ^! C
                  U    I
 ai
t-<    O
u^    2S

S    3
 d)  60

f-l  O
                                    VJ CO
                     Or-l          B
                     O   B         O13
                         OJ  01         *D
                      Q)  O  CO       O  C
                KtfljExfl    0)^(01
                a, 0,3     a) n 3 c  a.
                                                                B  B
                                                                4J  X
                                                                                                             a)
                                                                                                             B
                                                                                                             B
                                                                                                            X 
-------
      o
      co
      o
      CM
I
o
ts
 I
 Cl
1-1
1



g

£



§
M

CM
      (u
      O
                  60
                  C
               Or-4 .
            >,
         >-i  (J
         05  •      \O    t*1          COCM-*
Oey>OCT>OOOOO">eMrH
                                        i-iO

                                        do
                   0)  60
                   C  C
                           "O
                      C
                   rt  rt  « AJ
                  A!  a)  pa  a)
                  r-l i— I    CO
                                                                                v£>
                                                                                \O
                                                                                OO
                                                                   IOO
      a)  (lO
      B  C
IA    -H ^-t.
O    <-<  B •
CM    cd    OO
                £
                I
                             0°
                                  ffl
                               Q)  CO
                          ! 33  k  «     co

                               JJ  M  01  l-i
                                                             0]
                                                            t3
                                                          C3 •*
                                                          Or-l
                                                         JZ  O
                                                          h CQ
                                                            •D
                                                          U B
                                                         4J
                                                         B
                                                         0)
                                                                         >
                                                                         a
                                                      se
                                                                               S
                                                                               0
                                        D.O     B C  S E Q)
                                        co    t-i'vi 'CD  O O
                                        O4JuoJtoi-iPa
                                           O  OB M JS JS O
                                                                                           a>t-<
                                                                                              a)
                                                                                           o  >
                                                                       137

-------
•o
 S   •§
 §
               O
               O
      •o
       o»     u
      4J  >,u
       ttf-4  to
       o>*J,  tss
      go*
8    g

>
          00
              S      3
                     0)  60
                     B  C
O
CM
                    r^ C to
                     qj 0) C
                       flJi-l
              o
            JJ
      tO    B
      c JJ ra
         E O
         0>-r<
         O.U
      OCO J3
                                                                                   CO PI
                                                                             CM    COCM
                                     \OOOOOOOCMOVOOOOOOO

                                                      CMr-l
OO OOO
                            cP
              g

              S
      a
     •o

   Ot-l
  J3  O

   id
  vo
     •D

tO^-l  0)
                                         ffl ra >s
                                         eosB
                                         iJWO
                                      ao    s
                                                                        at
                                                                    i-i  >
                                                                     n)  cit
                                                                    •u  x
                               0)
                               09
                               0)
                                                                           _ _
                                                                           E E
                                                                     e  e
                                                                                                             01
                                   01 (0
                                  B  N.o
                                                                     B  Ot-i (8 -Bi-i  0)-
                                                                                                                  0)

                                                                                                                  0)
                                                                                                                  01
                                                                                                                  o
                                                                                                               CSO >>.C
                                                                                                                       t)
                                                                        138

-------
               4) 01
               rH 0
                  a •••< «i
                           I
                                                                            CM   en
                                                                            rH   O
                                                                            oooooooooo

                                                                            oooooooooo
            §
                  0)
          411
     w  >y.u
          CO
                 fi°;
                      s
                                ,3-            rH      CM


                           p CM O 1^ CM O O O O O O O O O O

                           CM     CMrH

en
O
CM
~   ri
•o
 I   I
 4J

11
O   U
 4)    £





 ^    £


      >H
     eoe°o
   4J B cd 01
r- c f< o 4.1
O . 01 5* «r* CiJ

° W*2 .0 H
        » a
     4J B «S
1^   B »* O
O   0) ?•"••!
CM   cua tj

     M,S1I
                     60
                     6
             cS     S
                   0) 60
                   B B
             en   T( tJ  0)
             O   rH B  «0
             o)    « «  a
                           I
                   (*.-»r~O

                   r^ooeMO
            oo
OOOOOCM
                                                                       OOiH
                                                                o«no»-iin
                                        r*.
                                        ooooo
                                                                o-*
                                   OOOOOCM
                                   oooooo
                         CM
                       JrH rH

                 OCMOOC5
                                                                       gvocn      O
                                                                       oo oooooooooo
                                                                                    rH   rH          rHrH
                                                                            •tf   \O O   O          O O
                                                                            r«-oo oooooo oooo
                                   en
                >1
               s
             O OrH
                     B U
                     0)«H
                  ǤM1
              s
                '
                                  SB!
                                         01
                                       01 CO
                                                   CO
                                                   •o
                                                 B-rl
                                                 OrH
                                                £> O
                                                 V4 CO
                                                 CO
                                                             cd «
                                                 U B
                                              CO f< 0)
                                                             0)
                                                             CO
                                                                           £
                                                                  BE
                                                                                  01
                                                                                  §
                                                                                  5S
                                                                                  01 BNO'
                                                             B OrH OJ  BrH Ol CrHrH
                                                              -  .  -. _i
                                                                                                  «0
                                                                                                                .
                                                                                                            M 3  U
                                                               139

-------
         CO
         m
         CM
                   60
                   Q)O
                                g
             0)  to
                t)   .a
                  0.1=
                C«r) IS
                Cd hir-<
                MHca
                                of
                                Q
                                                                                        o o o o o

                                                                                        ddddd
                                                                                                                            ooo
                                                                                                                            odd
VD
OO
O
    s
 a    t-t
H    B3
u.
o
   §i-« O C C
   cd-<-i K
                  0) 3 Sj3
                 CS O O 3
                                             •-<       oooooo
                                             o
                                             CM
                                                      OOOOOi-f
                                                      COu-i
                                                                               OCOvOi-lOOOO
                                                                                      l      O
                                                                                                O
                                                                                                O
                                                                                                O O \£> CM O rH i-l

                                                                                                d d -* ro d d d
                               OOCM
                                                   CMr-<
                                                   COCM
                                                     oooooo
                                                       ••••••
                                                     OOOOOO
                                                     o\o

r-4
CM
CO


toe
u c a
C *4 CJ
ei Kv4
o.a M
CO 14 *O
5

>H
«
Q


oom
CO



ino
f-i ta
              w e^

                s
                      oooooo    oo«*oo

                      "•» ir> eft o O t-i    OOCMod
                                                                                            a.
                                                                           to         -*    o
                                                                           CMOO oioo o
                                                                           ddddddd
                                                                                                            .OOOOOOO
                                                                                                                V    V  V
        M
        g

        a
        EU
                                          O
                                         .-*

                                         6
                                          o
                                             JJ   .  0)
                                             .o  e  co
                      a.0.3
                           JJ
                      B B  «
                                                        DO
                                                        »O
                                                     CT<
                                                     Oi-l
                                                     J3 O
                                                     |J CO
                                                     14
                                                     O-O
                                                        •O
                                                     o c
                                                                            c
                                                                            01
                                                                            OS
                                                                            >
                              •H-rHO.CC
                                                                  ,
                                                orotJ O603BOB33
                                               -                OT-13M^IP
                                                                B e-~<  B  e S
                                                        0,0
                                                        CO    i
                                                                                 CO
                                                                                 0)
                                                                                 CrH
                                                                                            01
                                                                                            C
                                                                                            a
                                                                                            si
                                                                                            jj
                                                                                            01
                                                                                         a) o

                                                                                         ai o
                                                                                         Ni-l B
                                                                                                                01
                                                                                                                •O
r-( 0)
 (8 4J
42 C8
                                                                                                                   C  X,
                                                                                                                                 01
                                                                                                                o)  a)
                                                                                                                e  o
                                                                                                                «  >j
                                                                                                        a>ooe-*,c
                                                                               isz
                                                                                                                         (U
                                                                                                                         c
                                                                                                                         (U
                                                                                                                                jj
                                                                                                                                01
                                                                                                                                o
                                                                     140

-------
VO
00
O
•tf
                   S  60 JJ
                i-i O  B fi
             O 0) f-l f-l 0)
             O S i*-l

                H w  «w
•o

 §
 B
f(
 JJ
 B
 O
 O
I
•-<    o
CM    2
 I    M
>    jj
      Oj
 0)    S
?—l    ^G
-D    W
 <8
H    g
        o s*5
      B 60 JJ
      O C C
       'a)
      m,*! 3
       I Qi-l

       ! S^
       I CQ t-l
      DC   U

    i S  ""S
CM h JJw) O
CMM oi  3fl
f> o i-i  ra U
   0) 3  S JS
   Oi O D 3
                             OOCMOOCM
                                          CM
                                          o
                        &
                             oo-*
      %
              JJ B  «
              C f-l  U
               acs  t-i
                                                                                                             COO30O
                 •c
                 0)
              JJ N H
         O    4)fl fl)
         VO   r-i C J.I
         <-<    CO'
                 S
                                                                                                              .   i intnin
                                                                                                             Oto OOO
                                                                                                       OOOOOOO

                                                                                                       ddddddd
PLE POI
                              •t-l  0)
                              S S H 000
                                                               141

-------
      vo
      CO
      o
      •3-
      g
r-<


>    I
                    e  to iJ
                 r-l O  C C
                 tH*r1*4 0)
              o E to,*: 0
              O Ui-l  fflt-H
              •* Of 3  OJ«H
                                                    CM           in
                        CNCM      r-»               o   tnr-«   o    r-<   cr.
                   OOOOtnO-a-OOOOOOOrOrHOOOOOOe**
                      O r-l IT> rH i—* i-M t— I
                      ooo<-
                                                                          a a
                                                                          •U X
                   01

                   ffl
                                                                                                                 01
                                                                                                                •O
                                                                                                                fl
 01
 4J
 0)
t-l 0)
 HI JJ
£ CO
 4J(-H
                        OI-Hi-l i»

                        §-gC
0)
co
0)

CO  0)
         4J
<-H       0)    O
 Cd    0)  O    rH   ^_  _
 •u    B  ij    js    ax:    >H O  4J
        41 O  _
        > B  N O
4JJ3 1-1  eg
wjj.ee
                                                                       142

-------
     o
     r->
     O
     8
                   tn
                                     '   IA   ,1—1    t-( 1-H rH i-« O
                                     i-HCM   OCOOOOOtO
                                     OOfMOmOOO< ---
                                                                                                      Or-I
                                                                                                      OO
                                                                                                         OO
                                                                                                             IOOOOOO
                       DOC
                       C 03
                    4J C
                    01  S <
                    Curt
                                   veooooo
vOf^cM OO O
     CM    V »>,i-li-
-------
      o
      r».


      §
1
 3   5
u   e
I   *
~   *
N
C«l   O
i   S
F-«    a;

g    1

      fe
      ><
                 •-< O   J£
                 •rffl CXB
              crv.ue.HC3
                « « llr-4
              rHr-< OOH tq
                                        O

                                        O
oo

do
00,000000

dopppodd
"    i
CO
                    
                                                                                         I JJ 0) 4J-O
                                                                                        01 0)r-l 0)-H
                                                                                       r-i i-» a. a jj  o>
                                                                                                                    d)0)BO)
                                                                                                                    B  B B) B 0)  0)
                                                                                                                    ra  « j: « c  e
                                                                                                                   £ £ 4J XI 0)  D
                                                                                                                   UJJWUM^-f
                                                                                                                    o)  o)
                                                BCB
                                                                                        o  H a B
                                                                                        W  OJ 5 fflr-l
                                                                                    r-l  S i-l i-S ,3  O
                                                                                     o  iUja e'eiio-
                                                                                                     f
                                                              0) u
                                                              4J 4J
                                                              a «
                                                             r-i i-i
                                                              « at
              H
              S
             CU


             to '
                                                                                   144

-------
     o
     r-.
     o
     vo
     CO
•O


 1
f>
u
 a
 o
o
i
                 1-1  O    J*
                 wl i-l  Cl.fi
                 4J  13 «rl CS
               * CO  (0  Wi-<
               l i-l  60H (O
                                                                            OOO

                                                                            odd
      i
              o
              CO
              o> si
              O O.U
              hi-t  (U
              3 O 4J
oooooooooooooooooooo
              tri
              CM
                         4J
                       00 C
                       e 
-------
            O 0
                        CUE
                       -H  18
                   - SJJJrH
               rH rH tCfH CO
                  O
         O> i)
         O\ ej
                                                                                                \O rH   rHrH
                                                                                                OO   OO
                                                                                                ooooo

                                                                                                ddddd
                                                                                                                        VO
                                                                                                                        o
                                                                                                                      ooo

                                                                                                                      odd
O
c-
o
AJ
co) a
8*H 3 O AJ
•O »"H JJ 0
5B M
M H
-
0)
Q
§O
OOCOCOO
-cMoOrHOO«n
CM v v «n
oo
oo
OOOrHCNOOO
OOOrHOOOO
                                                                                                     O\   00<£ r- *
                                       OO
                                                                                       V£>
                                                                            IT) rH       00
                                                   OO       COOOOOrHrHOOO   O

                                                   oo       ddsorHoddddd   d
              •o
              Q)
                                                                                                                            oo
O
CM
 60

M  M

"35
 01  M
                                      OO
                              COCOOOOO-3-OO
                              VDVO\O ooiDi-t
                                    CM V V
                                                                oo
                                                                do
                                                                                   O>   rH
                                                                        OOOCOroOOO
                                                                                              ooooooooooooooooo
                                                                        OOOf-IOOOO
                                                     CO
                                                    •o
                                                           o
                                                          CO
       M

       S

       UJ
       to
                                                                 0)
                                                                rH
                                                                 3
                                                             rH  >
                                                              CD  a
                                                             u  X

                                                             ££
                   OrH AJ

                      AJ  . fl)      T3
                    V  O B EC       B
              KKMHBtd    coo)
              oj a)  )j  ra B >,         HP
              gH«fl)«O-oo3Seo    S33
              P3M*O*D   «-1^^p?(3666rHrH
                                                                           S    00
                                                                           O    S3
                                                                           BrHlH.rl
                                                                           03 0) BrH
            0)

            CD

            AJ
            0)
         0) O
         B lJ
         S R
                                                                                                                  0)
                                                                                                                 •O
                                                                                                                  O    U
rH rH 0)
 CU (d AJ
   ^^ CO
   AJrH
                                                                                                                                           a)

                                                                                                                                           0)
                                                                                                          OWrH
                                                                                                       S    C
                                                                                                                        Q)
                                                                                                                                           "OJ
                                                                                                                                        * •  V «M CM •—^ ^^ ^— *»• B  Ul  S  O
                                                                                                       SrHrHrHAJCXil  I  Q)AJO>AJrH*rH
                                                                                                       ' -  '  - 0) a CM .rl -rl (3 X! .0)  O .rl
                                                                         146

-------
    o
    t^.
    o
•O   &H
 4)
 3   S


 '   I


 I   g
CM
CM   O
 I    25
>   I-l

 0)   04
     e
     S
w
               0) CO
              t-l O   Jrf
              •rifl O.S
               oj B«* id
                 j.-i
                 BOH «
CM
                                                            o
                                                        ooo
                                                                    ooo
                                                                              00

                                                                              do
                                                                          oo

                                                                          00
                                                                                        oooo

                                                                                        dodo
o

d
                 JJ DO
               i  o B  1-1
            co s «di-i  a)
            O O 4->f-<  4J
            CM z e o  «
                 oo*
                •oo
     wcoo
, ,-!    ,     oo
to   mir>  oo
>ooc«joooo-
                                t-iu"i            "">
                                cor--     CM     r».
                                oootoooom   oo
                                       ---  "
                                                                                       cMr-
                                                                                       0-40
                                                                                     O O O O O OOOO OO
                                        o
                                   Oi-l -U
                                   O   ffl
            £
          01 O B
     SB a: h H a
      a. D.3   <
          JJ  -
      e e a o>
                                                 CO
                                                 •o
                                                                  0)
                                                                 •O
                      03
                      JJ

                      5
                  •o
            0)     "O
            co      B
            eg   co 01
            0> co 3 ex      S    *
           •LJ 01 M eg >.   3   8
              " O 3 6 O i-l B 3
                fl CO O -H »-l 3 -i
 _   0>i-4i-li'£Via   S B i—I i-l B
i-i^ia,B6   ocor-i^o)>>ao
 cxec3o)f-<3oj-)4jcou'oi-i
M«.«*j^!H*!g.5^«3g3
                                                                               o
                                                                              f-H   8>a>
                                                                              X   J2  N
                                                                               o oi o  e
                                                                                   -li-lttl«e OJ2

                                                                B H « o PI-H o Pri w JJ jj \? p«
                                     •
                               s s: HOO
                                                                     147

-------
      o
      t^
*^
      1
      I
   4) to

   vH U   A!

   M«rl CX.B

O\ JJ B-»4  «
O» C O Pr-l

r-«i-< tOHB


  «5fi
                              OJ
                                                            oio-  •©•&••
                                                              •  »     •  •
                                                            oo   oo
                                                  o

                                                  o
oooooooo

oooooooo
                   U 60
             _i o d fc
             22  c «•** o
             O  O 4J«-4 U
                   e o «
                                                       oooooooooooooo
OOOOOOOOOOOOOOOOOO
                                                                                                                                                                  0) 0)
             2
             1
                                                                                                4J JS  «
                                                                                          4J 4J 0) WO

                                                                                           ft) 0)r-<

                                                                                          r-li-( O. 0
                                                                                     0)
                                                                                     a 41 n
                                                                                     « B B
                                                                                  4J JB 0) 0)
                                                                             AJ 4J O) 4J rl
                                                                             - <
                                                                                     e6jc.eo.fiO os
                                                                                                        i-i o
                                         « OJ= QO O O D
                                      VO ljf-40  I  I  I  I
                                                                                             O 0.4J SB S I  I  B
                                                                                             O «Tl  I   I -*VO  I
                                                                                 148

-------
    o
    f-
    o
    VO
o
Sv
                 a> 09
                      CuC
             er> u  o-H td
             e^  ed  cd Mi-!
             r-ii-<  OOH «
                                                                                      oo
                                                                                   ooo
                                              ooo
                   JJ  CO
                 I  O  6 K
             (O  C  <8-rl  m      ui   i/i
                        O o    OO      O   o
                         - —joooooooooooooooi
                                     0)  (1)
                                     4J 4J
                                     cd  «    o>
                                    r-l rH ffl 4J 01
                                     «  td 4J « C3
                                    JSJ3 «r-4 fl)
                                     JJ 4J«-< >B<    6
JJ JJ   rH Cd

3 Of-l  >>N

pa O >>J3 6
 I  I  42  U fl>


 i  i  0)  B  '
, I   i ,^ j ^ I ^g

Q Q O OrH
                 XJ  4.)
                 C  C
              0) (0  CD
              C Vi  Vi
              w   £
/-s O^"* 0) JJ
 ed N Ji! B J3
^ B^  pa o <
                                                                                     149

-------
        Ov JJ B*ri S)
        Ov a a lirH
                                                                                        §
                                                                                         CO i-l
                                                                                         oo
                                                                                    oooo
                                                                                        ooooo
                                                                                                  v
                                                                                                                            co
                                                                                                                            o
                                                                                                                         ooo

                                                                                                                         odd
o
r««
O

»
      B 0) O)
 O   -r-l AJ AJ
 C3   ^^ QJ 6J
 to   a o) a
                                                                                                     V V V V V V
 §   g
U   g
 c


!i
tM   Q
>   §
 O   Cu

g   1
          u
   •o .u   e
   01 B   (U
~ c 2   a
o •*( y o *-*
oxir-i ±1 a
C4 BO-I   0)
                                                                                      
                                           OO

                                            58
                                                                                eon
                                                          oo >A to oo o r>» co
                                                          OCMI>vOOOr-_'*_/>_.
            TJ
             ei
       o
       C"t
                           vDcooooocsioooooooo
                                                                                             OOOOOOOOO

                                                                                             ddddddddd
       o
       eg
               00
        i-l U
        (3 JJ
        a) ei
        B3:
                      CM


                       >!
                                   oo
                                 vO\O\OOOO>i-lOir>OOOOOt-lOOOO
£

g
W
                          o) o
                    S3 35 UH
                     O.G.3
                                      cS
                                      B a
                                                to
                                               •O
                                        o
                                        CO

                                        •a
                                        •a
                                        B
                                      CO 0)

                                      l-i to
                                                     4J


                                                     0)
                                                         l-H >
                                                          a) «
                                                         •u x
                                                       ,e. <=-d I

                                                     p B >j a ji j: o
                       01

                      1
                                                                                     a
                                                                                           01
                                                                                          •o
                                                                                           M
                                                                                           O
                       0)
                    01 O
               •U   Oh
               o   01 o

o,              H   27!



5 *^? *!!J *T.    ITT "» 2" X /"
to  O/ c t"'    O O 0) W r™
60% 0>rjO>BMOI»-.^^
BPr-ieBt-IO)BT-Hr-(i-l4Ja.«
                                                                                                            01 01
                                                                                                            U U
                                                                                                            « a
                                                                                                            rH r-l 01
                                                                                                            a a u
                                                                                                            £f a
                                                                                                            4J Ui-l
                                                                                                                 ra
                                                                                                                    0)

                                                                                                                    0)
                                                                                             ... w
                                                                                             u o
                                                                                                          B KI-I
                                                                                                          o«!^
                                                                                                              0) (U M
                                                                                                              c ij o
                                                                                                                         0)
                                                                                                                 ra to
                                                                                                              _
                                                                                                          -i-H e J: ai 6 i-i
                                                                                                      «   O ^ pi,gi S H
                                                                  150

-------
•O
I
    o
    r«.
    O
    S
    g
4J
B
O  <
CJ  EH
    £,
CM
CM   U
 I    Z
>   H

 0)   BH



|   *

     fe
     3
     en
0) CD
rH U JA
•rl-rl CUB
OX 4J B-rl «
ON S) <8 HrH
rH rH 60H «

0) Q)
O OflrH
ui is e.
MM
"§•0
6 01 0)
O *H 4J 4J
co iSS
4J
•o 4J .a
0* B 0>
O «rl 9 O 4J
©.CrH 4J B
CM s>w o)
8S rn
4J 60
O B rl
1 SliH 0>
CO C 4-1 rH 4J
O Pj C rj at
S*Jg*

01
B • fl)
CM "rl ? 4J
CM EJ p£ ai
o *
u
60

rH rH 0
O Ot 4.
CM , . 01 «
CDS
B






£
M
2



Cu
^

CO
^
at
O

CO
I

CO
I
CO
I
O

CO
S*
e

CO
ca
Q



CO
>•
01
a























^oHoc^oooooo^ooo
CM V V CO
OO VOrH CM
OOOOOOOCMOpOOOOOcoOOOO
(AOOcOOOOrHOOOOOOOOcOOOO©
CM V V CO

I-H rH
in CM o o o O-CM ooooOrHOooocOf-i

CM V V rH U"»CM
rH

ci ^y*' CT*'*A '' ^^ f ' '
CMOO\OOOOOrHOvt>OOOOOrHOOOO<
CM V V



So m m
OOCMOOOOOOOCMCMOOO
OOOOCOOOONrHOr^OOOOOrHOOOO
CM V V rH


O tn 4J
rH "O fi
.£* »rl O)
U rH rH
o at
O M rH >
Oi-H 4J <0 0)
o at "O 4J x
4J • 0) *O O Ol
0) O B ra B H K
K EC MH B « coot
(i. Cu 3 < 01 M 3 O. •>* 0)
4JM ^|0)r(CI9p% Be CO

Pgtl*rj»rj •*H^!COO'r*3"tH"fHV( BrH
B B 0)  • O
01 0) O rH
4-1 B fc J3
o oi o u e
H NrH B (
fi J3 l-i 0) <
SB •> 0>OOBr

•rl -rl MrHCOlHOrHJ
BrH 01 O 01 M EH rl >>4
0)rH 0 •> B N O^^O^J
Q)J3«tH"*H^! Ol^rH^C OJ '





vO
o
o
o

tniri CM CM
CO OO rH O
CMOOOOOOO
oooooooo
V V
iri i—t \nin
§o oo
ooooooo
oooooooo


CM rH
o o
ooo
OO 0


oooooooo





>oooooooo
>oooooooo



0) 0)
4J 4J 01
a; at B
rHrH O) OI 01
CD at 4J rH B
£if a) >•> oi
4J 4JrH ^3 i-H
UrH 4J CO 4J
3MrH,C!Ci>Q>rl O>
) 0) >.Pi B IH O O
H ,£ 4J 0) .d rH IH

MfCICQ ^lOt B O BrH
j 4*J i *B Vi at as o *C
Ll 1 O> 4J O> 4J rH -rl
JCMM-rl BJ3 OlOtj
                                                             151

-------
      •o
            d)

 !-•    elf* n
 -*    a) —) a
              O    JJ
                                      OOOOOOO
                                           i-H      O
                                                                        CM
                                                                        O   .*
                                                           OOOOOOOVDCMOCMO

                                                           mvooodddddddd
                                                           •*-*
                   •O
                    0)
                    e >.
                   1-1 i-<
              CM
                    o
                   o
                         OCOOO OO
                                                                        o   VOCN      .3-
                                                           OOOOOOOCMCMOCMO
                                                                                   CMO
                                                                                           CM   O    O
                                                                                           0 _ O _  O
                                                                                                                  CM
                                                                                                                no
                                                                                                        mui   oo
                                      O
                                      o
                                      VO
                                                                                                OO
                 o>    CO
                 03    C
                 eit-i-H M
                    CVrH 0)
              o e  a> a) *J
              CM in u a) o
                 e) co o

                 "
     o
     r»

     §
                      CO
             o
             CM
                                                                     OCM
                                                                                                             o   o
                                                                                                vO   FH      O   O
                                                                                                CMOOOOOOO
                                                                                                                        00
                                                                                   OOOOOOOO    OO
                                                                                                                                          o
                                                                                                                                          o
                                                                                                                                     OOO

                                                                                                                                     odd
     e
CO
CM   <


i   ^
     z§
J3   2
 H   HI

H   £
     co
     Iw
     o
     JM
     5
     CO
             8
      •a
      01    B
      c a  «
      •H U  0)
      ^3 O  M
      H a 4J
         O 0
CM    a jj jj
o   1-1 e to
CM    jj 0) a

      an
                      u>
                      c
                     Tl 0)
             r*      r-t 01
             O      J! H
             CM       0 *r4
OtrtO
 •  •   •
rHCM O\
                                                                                                               OOOOOOOOOOOOOOOO
                                                                                                                                  O   O    OO
                                                                                                                                  ooooooooo
                                                  oooooooo<« I^COCM ooo

                                                  OI-HO VOCM o o di-< com d dd d
                                                                                                                                             OO
                                                                                                                                     OOO
                   4) 09
                   U CXW
             O    UT-( 0)
             CO    3 O 4J
                  W
                     X
                                                                                                                 lOOOOOOOOOO

                                                                                                                            >odd odd
                                                1H
                                                O
                                          OrH •
                                         o   a
             M

             S
                                «
                              MH
                        Cuo, D
                             4J«
                        Baatu
                                                           Ol-H
                                                          jz o
                                              a
                                             o-o
                                                B  n)    co T-I Cl
                                               <  0) CO p c D.
                                                     0) C a co
                                                                          jj

                                                                          0)
                                                                        a a

                                                                        o a)
                                     i  a
                                     •HiH O, B


                                     SSH1 O
                   p c D.         -  -
                   C a co  X       B H
           cuwooeosnoEsa
               i-i fi LI tn  o •*> s -H -3
                u  0.0    E c-S  a B
           C    Oto
                                                  O tn.ti. HH«ooooi-HH3SScoHsityDSl
                                                                        BrH MH vt
                                                                        a  0) B rH
                                                                        eojd a) i—i  o >
                                                                        B  OrH a  BrH
                                                                        a ft o> ,c IH •!-< j-
                                                                          •~ WH  - " "^
                                                                          152

-------
      o
      r^
      S
•O
 01    JB
 9    O
 B    pi
i-l.   Cb

I    g
O    «S
CO    O
7    g
>    £
5    I
1
      S
                     •o
                      01     a
                      C  0)  81
                     •<-<  4J  01
                     45  BJ  M
                      e  a  u
                                         ooo
                                         6©o
                                                                  OOOOOO-*OrHf>».tU">OO©OOOOOOOOOOOOOOOOOO
w.
                     "S-OB
                      B  0)  0)
               O    -A  U  9
               O    .O  «r-<

               "*     o  2>w
                     OHM
                                 8
                                       in ooo
                                                                                                                         )          rH       rH       ITIlfl      O
                                                                                                                         >          o       o       oo      o
                                                                                                                         >ooooo oooooo ooo
                                                         r-H       CM
            •O 4J     B
             O)  B     01
         O  B  0)     B
         OT)  SOU
         CM .O r-l JJ  0)
                      01
                B     M
                     H
                   cSS
                                                                                    iri o O O O "1 O O O O O O
                                              U r-l
                                             0«
                                              OtOE
                g
                                  e  s  01 •* •*•
                                 1-lT-ia.EB
                                        i-t  •
                                                                                                                                          .
                                                                                                                              D a>n)o
                                                                                                       >  e
                                                                                                                                                   CU 01
                                                                                                                                                  ,    c
                                                                                                                              4J  41
                                                                                                                                           '  •"
                                                                                                                                          CM
                                                                                                                                                 '  B
   01

   01    01
   f~*    G
   >>   0)
   (£4    r™!,
   4-1    X
                                                                                                                                                  0) 1-4    01
                                                                                                                                                  MO    O
                                                                                                                                                  ffr-f    Vl
                                                                                                                                                  *J J3 01 O
 C  I-i  9  O
 01  U r-l-rl
JS  0)  O  IJ
                                                                                     153

-------
                 •o
                 O   O)
                 S >>4J
           O    1-lrH B>
                 ,
                 BO
                 o
                                     Oi-ioooo m
                                                                      CM              «*
                                                                      O    CM O   CM-*
                                                          OOOOOOOCMrHOCMO
                                                                                                             l-l   CM                                  rH
                                                                                                             O   O         wioo                      O   O         O-*           ir>ul    OO
                                                                                                CMOOOOOOOOOOOOOOOOOOOOO
                                          i-l      00
                                                        COOOOOOOOOOOOO
                                                           -
                •o
                 0)    0)
           O   4J  5>%4J
           M    BrH CO
                                     oo\oooo
                                   IDVOVOOOO
                                        rH      CO
                                                                      •£              00
                                                                      O      CM VO I-H CO
                                                         OOOOOOOcorOrHCMO

                                                         oWdddddddddd
                                                         rHCM
                                                                                                      CM                                   i-l
                                                                                                      O         U1   i-t        0000      O
                                                                                        rH            O         O   OO        i-l I-H      O
                                                                                   COOOOOOOOOOOOOOOOOOOOOO
     o
     r*.
     S

     £
                eg
                0)
                    CO
                    C
           CArH OlrH «J
           o B a>  B 4J
                 u  m ca
              SS W  C 3:
              U    C
              CO   <
                                     lOOOCOOOCMr-IO
 o
 e
     E
.
 '§
f>   o
CM   S
 <    M
>   J
     O.
 e   a;
A
£
     S
                    CC
                    C
                   •rl U
                   ft <0
                    es jj
                    Ct C
                    C*
      •o
      ey-o e

      §-rI 5 3
      J3 tdi-H
W    «
              OB    M
             O M   H
                                                                                                                                                      CM
                                                                                                                                                   i-i o
                                                                                                                            >O   O         OO   OO
                                                                                                                    o o o o o o o o o o o o o o
                •C 60
                 0) C
                 CT<  0)
           CO   -rtr-l 4J
           O   U3^  CO
           CM    BUS)
                UPu
                                                                      VO
                                                                      ro
                                                                                                     UV      O    O

                                                                                               ooooooooo<
                                                                                                                                            00
                                    o
                                          01 p B to      u B
                                    SS JB >J H B a    (Ofl Q)
                                    Cbd.3   .
                                                                       B
                                                                       0)
                                                                    id a
                                                                         '
                                                                                                   a
                                                                                                   w
                                                                                                   5
                                                                                                             0)

                                                                                                             a
                                                                                                            j3  01
                                                                                                            •u  B
                                                                                                             oi  a
                                                                                                          a) ox:
                                                                                                          a t-i 4J
                                                                                                          0) O  0)
      01
 01   -O
 C   *r^
 01    f-l
 3    O
rH   rH
 O 01 J3
   BO
                                                                       MM        CD
                                                         _           HB         OB|B

                                    33$-l'O*D   *rl.TJl>IC£>Q*r(3*lH*'Hh      C,-H»iH*iH«rf
                                    8 B  0) iH ^1 ; B  N
                                                                                                        NrH O S  O 0)
                                                                                                                               B  0) 01 
                                                                                                                               aiHrH i-H 4J
                                                                                                                               rH  a a a a
                                                                                                                               B.C.C.CI-I
                                                                                                                               01  u 4J u a
                                                                                                                                         JJ

                                                                                                                            B TJ  X >»rH ft<
                                                                                                                HhMNOlOIOQJNX
                                                                                                        o i  a o i
                                                                                 BqrHat)BrH'0)BrHrH!kirH  IJ34J 0,2 T
                                                                                 Sz!.o)IBrir|i-ix:  oijSrH oi^vou  o> a> CM
                                                                                                                                     01

                                                                                                                                     OI
                                                                                                                                    4J
                                                                                                                                  O) 0)
                                                                                                                                  B O
                                                                                                                                  0) M
                                                                                                                                  IH O
                                                                                                                                      Q -£,' a
                                                                                                                                       I  iJ Ij
                                                                                                                                          0)
                                                                                                                                          B
                                                                                                                                          0)
                                                                                                                                         I-H
                                                                                                                                          I
                                                                                                                                       Q)  Q
                                                                                                                                       BrH
                                                                                                                                               .0! .0 _M
                                                                           154

-------
    O
    VO
•D


I
v<
JJ
B
O
CO
CM
 I
 4)
rH
^>
I
o
5
E2
    fe

    I


IS
4) 4)
O JJ !».JJ
rH (SrH M
H

•O
41 0)
B >iJJ
O -rl t-< CO
CM SOS
O

B 00
co B
OJrHf-l rl
ON rH 0)1-1 4)
o B 4) B JJ
CM .rl JJ 0) «
« W B »
4J B
CO j ^3 C^ c? C5 CD CD CD ^5 co CD ^D ^D
\O VO COO
1— 1


CM CM r—
CM O moo CM
OmOOO OOVOOOO OO OOCMOOO
VO VD CM O O rH rH O F** CM O O O O O O O O O
r-




CM m ov r*i r**> oo
OOOAOOOOOCMOOOOOOOcMmO«3-co
voo'inddcMrHdeM^dddddddddd
rH rH rH tn


*
mvo
i*^ o\ . o co vo m -^ m
OO O.OO.O.rH^ CS1OO;O-OO-O O'rH r>COvOI»-OO
^5 C5 1^ ^5 CD C? '^^ ^5 ^— > C5 C? ^^ ^^ ^^ ^^ rH rH O^ ^^ CM
cMc>3ddd-*d'-!o-*odooo«*inrHoo
CO CMVO



M
O O> JJ
.-* r! *r! 0)

JD o a
O rl CO rH !>
UI-H jj a a a
o « o-o JJ x
fl) O B w OB H-'SB---
S3 pC IH B-I B a co'*rl fl)
JJ* rlfl)riatO>. SB tO
BSaO)0)O'OOt>03BOB33 4)
SSUtS'-O «rlJ3WCOO«rl3*rI*rlrl BrH
B S fl) «rl «H 08 }H CuO SB'HSSO) BO)
«rl.*rl Q4BS OCO rH»rl4)SOOO4B'O 00*Ai
BXEBBrH3OJJJJJJtO*OV/ v v v v


rH CM
m o m com coco o
rH O O CM O rH rH O
OOO OOOOOOOOOOOOOOOOOOO
 B
a 0) *O arHrHrHJJ 0) O)
j;o) B -ri r-taaaa r-i B
JJB 4) M B,B*B.Br-4 >, 4)
'rH 4>a 3 O OlJJJJJJa JSi-l
O fl) 4) O fl) JJ 6 S fl) frl rH rH J3 SO JJ
H JJ Nr-l O B O 4) ST3 X >>r-lpH 4) 4) rl 4)
§fi »B 4)OOOJJBBr-4Hq-4a)4)aoxo)o>^ojJj3o)o
BrH (UOO4)rlHOh*rlrH>.JJJJJJrHlJJriaaUj2
*«i 25*Tj ri"£* m'r'^l m'r'vo'S'm rt*^ eM^«rl«S^-emo IH
                                                             155

-------



















«*
>
9)
rH
J*
H



































CO

1 1
S
e
i

u
2
S
i


o
i
i
co

















o\
•a-
CM





O
rH
CM


^
O
CM


U1
O
CM




O
IN




CO
O
CM


1-4
O
CM






W
s
•1
0)
a.
05 CO 5
 B a
0) to O
BJO e
o
o
60
B
-H 01
rH CO
^ B
cw
•c BO
0) B
EiH 01
•rl rH CO
*O ^d B
H O«rl
0*
•o
01 01
B OlrH
•H U O
,0. to B
H a o
osw



u
B B
6 01
•rl U g
4J Cd AJ
3 01 «
rH E 01
0 M
CO H
60
B
•rl 01
rH CD
v B
0-rl
S0*
•O
oi a
B 0) rH
•rl U a
,O H> B
B a aj
O ^C C/3
o









rH
>

C




rH
S)
Q


rH
Si
Q


rH
O



rH
^
S)
a



rH
a


1-4
ffi
O









00
u*l O fl ON CO
cM-3-o "xj-cooo OOOCMOVO move

CO VO OO rH rH
CO •*
rH


VO rHrH VOf**^*^
CO CO O rH CM O O O rH O CM O\ r^ CM O
CM CM O rHO OOOrHCSCMOOOrH
CO CO


„_ OO mco CMCO r^ €»•*
CO CO O O O <3" VO VO VD O O O CO O "1 O O rH ITi
CM *ij" f^t O O rH r-l CM fl ^ o O U"1 O CO CM O O O
CMVV rH ~^,v-.w.v-i-H04
C>) i^ ON O O ON ir"i O O O O 
COCMO OCO OOOCOOCOrHCOCMCO
U1 CO

VO C-
00*H; CO rH CO ON t*- ^* VO
OOOOOIAI-. O OOrHOSOONCMO U1
o o o oo o CM dddeNdd
CO


O CO CO 4J
£ 33 S
0 rHrH rH
O O 0}
o°«S "" SS
u • a) "o > o 01
OlOBco BrH H S3
aSSChHSffl cooio
o.o>a§O3^>> EB ™ IS
8§01-rl'rlvi$|JOi BB-rtSEO) CdWBrH
•HIHO.BB ocorHrH^iosooa.B'D aoi o> i-i
5i5^2Sri52'y'y4joi'ciiibcL'onic!t>'~<<«
•rl CO 01 p% >>*H rH,COOBMCO.C.BOlHO!cO«rl01-£
SSSHOOOfaPuHE-i^^CJOOOrHMSCiSCOtH


00


*•!•

*

'

VO O
cod


ooo
CMOO
00
,

§00
o
CM



_ rH IT1 rHrH rH
ON O O -4" OOO
••••••••••••••••

V

vO

OO
VO O
09

1 	 , . .
1
o'oo
r»-OO


' Q)
i 0) U 01
, B 01 CO B
CO tJ rH 0) 01 0)
•B *rl Cd 4J 1—4 B
J-> IH .C « >> O)
rH 0) 0 CrH ^. rH
i CO 01 O rH -fl-cd- • 4J >,
4J B (H X! 0,^3 01 OJ .C
O O1O UO)rH4J BO U
H N*i§ BX£0)0)»H 01
*• 0)C)OBrH.C Ol-CrH Lj
co o) js «ri «« oi n) >M-H u u x; oi o
0>BNOl O4JJ3W4J42BM90
BrH01BrHrHrH4JCL
-------
             ON
             i—I
             es
                     X  «
                      O CO
                     a
                                            OOOCN

                                            dddd
                     O

                     O
00

do
                                                                        O O O "I v£> r- O
                                                   OOOONOOOO
                                                   o    i   •  "
                                                   ON    00
                                                                            OCOO
                                                                              •   •  •
                                                                            Ot-lO
                 V  
                   vl U 9
                   US  Wfl
                    e  oxw
                    O  tH<*4
                   OH W
                                            oo
                                               O
                                            ve
                                         CM VO
                           OOOOOf-OOCMCM
                                                                             OOOOOOO
                          01
                    0) CO  JJ
                    coi-<  (0
                    1-1 CO  0)
                    (DOB
                    > S  M
                    (1) M  01
                    oio  a.
                                    tr)\DOOOOcN"">O   OOOOOU1COOOOO      VOOO
                                                                dddddr4oddd      csod
4J
e
O
CM
 I
 01
rH
A
                    0) 00
                    6 C
                    •rl-H  0)
              rH    rH B  05
              O    eg «  e
                       0)«rJ
                                                                                                    V)   POVO1TI
                                                                                                     p^ooo
                                                                                                                     VOf*.
                                                                                                                      odoooooooo
                 i-H "O 60
                 «-<  01 C'
                >  <8 4Jt4 0>
                 -H  W i-l 4J
                 w  a) Ji os
                  H  U O «
                                             •*•*
                 rH T3  60  '
                 rH  01  B
              CS  OJ  4-1-rl 01
              O -rl  eOi-H 4J
              CO  JJ  01 r^ tfl
                  rl  rl  U «
CNVOO

    •VO
      e>i
                                                      OOOOO OOOf
                                                                       CM CO CM    f»CMCO
                                                                                                  00
                                                                                                  •Jf
 01    0)
 B 0)rH
ft 4J a
A to 8
                                     mooo oo CM ON ooo
                                     ^•vOenOOfOOOO
                                           en
                                                                 OOOOOOOOOO
                                                                                                   Sgo

                                                                                                   rHOO
                                                                                 00

                                                                                 do
               H
               g
                                      JS35
                                                 rl
                                                 O


                                                 O

                                                 O
                                           O rH 4J
                                           O   (0
                                               4J  • 01
                                            m  o C co
                                              H § ffl
 co  co
•O "D
•rl-rl
rHrH
 O  O
 to

•O-D

 BrH
                                                                             §
                                                                             rH
                                                                             CO
                                                                          rH >
                                                                           a 03
                                                                          •u X
                                                                               01
                                         e eg
                                      iH-rl

                                         « 0)
4                                eg    co a> O
                                0)  CO 3 S. co
                           -    p  0) rl CO CO
                          o) o) c -^ ~ ~  '
   a>


  1.
   0) eg
a)  ox
B  U JJ
01  O 0)
tOrH O
                                                                                                           01
                                                                                                           4J
                                                                                                           eg
                                                                                                          rH  01
                                                                                                           eg  JJ
                                                                                                          J3  eg
                                                                                                           OJrH
       §•§§,-,
                                                                     B*rlS
                                                                        BO
                                                                                 B.C'O
                                                                                         0)
                                                                                         co    e  e
                                                                                         oi    3  s
                                                                                         CrH-rliH
                                                                                         C8 0> CrH
                                                                                         OOJl! 0>rH
                                                                                         C OrH  (8
                                                                                              01  -C
                                                                                              WH
                                                                                                                         -C     ax
                                                                                                                         O  0)rH 4J
                                                                                                                       B    B  XXI 0)
                                                                                                      0)
                                                                                                      B
                                                                                                      0)
                                                                                                   0)  01
                                                                                                   B  O
                                                                                                   0)  rl
                                                                                                                          0) 03  >M-I O 4J J3
                                                                                 O)

                                                                                 0)
                                                                                                           0)
                                                                                                           O
                                                                                                           rl
                                                                                                         0) O
                                                                                157

-------
    CO
    «n
    §

    g

,a

II
AJ

II
  g
43  CO


fl  fe
             oi m

           SJ-rl-H O."5
           O\ U Ox-l B
           tH B «8>liH
             t-l 60H CQ


             ££
                                                                          OOO

                                                                          odd
                                                                                                 oo

                                                                                                 do
                                                                                               o o  oooo

                                                                                               do  dddd
               o
          o
          sr
StH'tO
o—i B
£0*
                                    CO ON rH CO
                                    ooo r-»m
                                    ooooi^-
                                otoooo<—
    m  rHiniHtH      ' r^
 -  -01  O«NOO  m   o   eMn
cMno  oooo  co   o   oo
        	>oootnoooo<
                                                                                             m
                                                                                             o
                                                                                              m
                                                                                              o
                               CM     i-H
                                                                                                                      i OO
          §
CO B
BUB
t> »H C O
r-lr-4 -H
5f^ O.M
O C042
« 3


rH
1


n
                                                                  CM
                      10
                      O
CM
O
in
O
                                                                                                           in
     0) B
_    O O.U
O    t*«H 0)
CO    SOU
f«    O-r4 B
                      I
                                mm
                                oo
                          CMi-lOOO
                              CNI eo I-H i-i in
                              ooo >nr^
                              oooof)
                                                             t-l  i-l CO tH tH      '%£)
                                                            -

                                           B B

                                           U X
                                           O 0)
                                                                                                    0)
                                                                                                    B
                                                                                                    O)
                                                                                                o
                                                                                                I-
                                                                                                          0)
                                                                                                          B
                                                                                                    ai

                                                                                                    B
                                                                                                  0) J3
                                                                                                  C JJ
                                                                                                a) co a)
                                                                                        a) a)

                                                                                      BBB
                                                                                      0)0)BAJBB4JM
                                                                                     .QNJSOIBJSaJO
                                                                                      OBJJOXliJOiH
                                                                                                                       0) 0>
                                                                                                                       aiai
                                                                                                                      r-lr-l
                                                            158

-------
     oo
     in
     O
     vo
                  0>  09
                        O.C
                  4J  C -rl  0>
                  «  ffl  Mr-l

                 r-l  60H «
O

d
                                                 o

                                                 d
oo    oo

do    do
o
d
00000000

dddddddd
•o
 §
 §•
P.
      IS
                     9)     fl)
               CM    i)  xu
               O    ffl r-l  W
               •*    CU-r-l  (8
                                                                                                      oooooooooooooo
                                      ooooooooooooooooooooo
JD
 CIS
      C5
      g
      52
      tn
      o
                     oo    e
                     C 4J  W
               VO -O-r) B  O
                  o«-i
                  CJ O

                     "
                                                                00
                                      OOOl
      5
                           4J
                  •O JJ    C
                  a) c    o)
               O B 0)    S
               O-H 3 O  4J
               C§§<
               s
               a
               a.
                              0) 01  C  tt>
                              EB«8Btt>4)
                              co ax  a  c B
                                    4J £  0) 0)
                                                                                                                                                                BBC
                                                                                           o  E  e e
                                                                                           to  «  (B tO
                                                                 0)    O
                                                                 C 0)  B
                                                        (D (11 0) "-< C  0)
                                               f-l
                                                O
                                      AJ  B  O  to
                                       4)  0)  6
                                       >>« j:  o
                                       e x:  B. 03
                                      •H JJ  O 4J
                                                fl)
                                          CuO  6
                                                        <1) ID
                                                        e E o
                                                        OO^
                                                        BMO
                                                        OOi-
                                                                                                                                                  ,
                                                                                                                                                    r-l r-l  0)  «  01 X!
                                                                                                             osuearioo'OfiO'-iot-ieo. &.4J u m n> o <*
                                                                                                                                                  Urln-l4J4J  B
                                                                                                                                                                         c
                                                                                                                                                                 i   i
                                                                                           .....  .	 _ _
                                                            '  '  *  ' H  '   I   I   I   I  I   ',CDt-iPOO4J4J4J
                                                                                       159

-------
    0) to
   •H O   .M
         0.C
      C-H ooooc
«*
CM
 I
JO
&
      60   B
      CUB
\D-O-H B O
OrHrH ftfH
C4 Qr-4 Q.M
   U OWJ3

     K   3
               •O JJ    B
                OJ C    0]
                §B o    a
               •n y  o 4J
            CMUir-t 4J a
                B>H    V
               85
                                                                  V    V V
                    89
                  O ft.
                  Ot-l ,4
                  MOV
                    B a
                    SDK
     c§
            g
            M
            2

            I
            CM

            CO
                                                             a
                                                             B 01
                                                             01 B
                                                               O)
                                                                                                               0)
                                                                                                                         0)
                                                                                                    ^•S'-N
                                                                                                    X W C
                                                                                                    O O nt
                                                                                                  -
                                                                                                  «         ^(
                                                                                                C M-l    0)    X
                                                                                        e>Hn-i  Br-i    -o    8
                                                                                        •  1 i-HW g    >,   &,
                                                                                        ftnt-. 3r-ICO    43    Iff
                                                                                         • « to  9      ID
                                                                                        CM CD O  to C    13 I.J M
                                                                                             O  O 18    rH O O
 0)
•H
rJ
                                                                                                                   ou
                                                                                                              _ _ « «-* 1/S CNI CO-3-VO rH „,
                                                                                                               i  po  I  iMCScseMcMtMOjs
                                                                                                               tdt  tdtdrHrHrHrHrHrHrHft,
                                                                                                               -  -  ~ 4J  I  I  I  I  I  I  I  (8 Ql
                                                                           160

-------


















00
o
vo

|
•a
§ §
c £
4J
B «tf
0 H
O <
^ Q
•* (S
CM Z
1 1-4
'"* g5
01 2
rH <
O3
H [n
S
Crf
E
g
CO























60
i-l 01
O^ ^i 03
O to B
CM (DiH
B f**t
£
T3 60
a> e
. B i-4 0)
r^ 1-i rH CO
0 J34 rH
O j£> co E

JrlcS








B
s
s.
Cu
CO

CM
•>,
03
Q


CM
^,
(0
Q


CM
cd
Q


CM
^
cd
O

CM
^
03
£^





CM
K.
cd
Q



CM
5»
cd
Q




CM
>
(C
0












C3> ^CO S rH
OCOOrHOOOC^rH-d-OOOOOOt-HOOO
vor^-cooomoocMoooooooooo
pH


00
o>oo mcM om-* r-if-
CMVDr-~OOCMrHrHCMOOO-*rHini-HOOO
CM rH


00
^ po O ^O O O OOO CO CO rH O O
CM 0
vO
CO

O\ m-«t O CM OOCMrH-*
CMinr~OOrHrHOVOOOOCOOOrHOOO
CM CM g rH


OO in r^- *^ CM
in i£> o O O CO O CM vO OOOOOOCMOOOC
vOv&CMOOCOrHOcMOOOOOOOOOOC
CO V V rH





CM
*H^ O\ 
O rH 4J 03 03
O 03 *O 4J X
jj . flj 73 O 0)
& O B 03 B H S
AJAWO)>-4n>> SB 03
|Bcd«IO)CJ>OO3CoB3i3 W
i-t*rlCXBB OOSrHi-ialBOOCXB'D 60Jl!
SSHOOObitwH^OOOOMJsa
in

i-HOQ



in
OOO
OOC5
*"^



CM m
OXOCMOOO c
COOOOOOC



CM OO
OOOO
rH


rH U > B N O '
rHC8S<-IO)S'-4rH


O
0









rH
CO
>ooe
>ooe



0
o



s
o
o














0
o













0)
01 B
B 0)
5 2
.C rH
oroet
'orm
troto
rHm iH
Si O B
U Pi-l
03 O C
XrH 1
!§ScM

O
o







t

m m
o o
>OfOOOOO
>Ocor~ oi
JJ 03 rH B
03 rH >> 0)
rH 03 ^3 rH

£ 4J 0) 0) ' ,C
4J .C BO 4J
jsE o> o) n o>
Cb B rl O O
rH 0) JSrH K
X£ 03 B O BrH
f u ij 03 cd oj j:
« B "S S JJrH^I
QS^£HHH
161

-------
    CO

    i
 e
•H
XI
-a-  o
CM  SB
 «   w
JO
5
0)
03 CO U
(Oft C
fr) t| GO d
O 0) o £
*^ S* Ei I-
•ScSrS
•O
0) 0)
CM U >,4J
O CdrH tO
>» o~-i s)
U0»
H
at eo
B B
•H *fH 0)
rH rH B tO
O S) CO S
33*
rHT3 60
i-H OJ B
\D C3 4J«tH 0)
 J£ S3
U M U ca
ai o>
C 0) r-l
r-< "-(.DO
o x> to a
co B ea eg
tSStw
0)
01 co cd
M B 4J
ON 0) O B
•* !> B 0
CM 0» W 0
050 B
O
U
co
e
_ -rl 0)
O rH to
rH J£ B
€^4 y ^^
a.


SAHPI£ POINT
CM
>
CO
O
CM
cd


CM
Is
Q
CM
«
O
CM
^
a
0
CM
a
o


CM
e)
Q




CM
^
Q

•


i
*^ CM
_ o> CM vooooN-a- o CM
Or^O rHOCJvvO r-4 O OO O VO 1/1 OOO OO O OOOO
<1* VO O\ O O VO rH O O OOOOOOOOOO rH O O
CM

VDIO ^ CO i— icOi— ItOrHrHirjr^fO
VOI-OOOCM rHrt OOOOOCMrtOOO " O O O O O O O O O O O O O O C
tnvo^oo^ dio dddddddddd ddddddddddddddde

' 	 : '• • ;;
tr>ir> , ,_i PH ^f r~- r-i
O\ O\ O O O rH O\ T-4 CO OO OOOrHrH OOOO OrtO OOOO O OO rH
IO V V ^H ^"^ ^"^ TT^ ^'^

U^ ITl 00
OOir» i-i m to CM to r- m
OO >O O O O *O IO rH CO O O O PO O 00 f^ C^J O C*) ^"* O CM *"* f^
CMCOOOOO«Si-(T-tjav oooooi-JOOOOOO OOOOC5 OOOOO i-*OC> O O


CO
CNJ too voeooooooo^o Ot-i mcoa\ oo
C*") ^H Ov in ON e*"i
CM rH SS^rS'>,£i5rH?
'W a>I~loS>CNO'SoCl >»x! £ "H W >,S5
zzSc^ogfifififi^^iSScjI'^l^cSlsSllfiSl^JSaSI'risl'si




1-4 -^ i^" I— 1  oooooo
V

VO VO i-l rH
i-H rH O O
o ooooo
d ddddd

























0)
0) B
fl) 4J m fl»
)iethyl Phthalat
Jimethyl Phthala
Anthracene
'henanthrene
!etrachloroethyl<
'oluene
?richloroethylem
                                                         162

-------
      o
      CM
       t>0
       .9*
       r-l  01

       U
                           U1V3OOOOOOOCMOOOOOOOOOO
                                CM
                                                                              VOOO

                                                                              does
                                                                                                o
                                                                                                o
                                                                                                            o
                                                                                                              •
                                                                                                            o
           •O 60
            o> e
            c-n o)
      fv   .rl r-4 to
      O   J04r-<
                 •rl JJ ft
                 ,0 co B
                  B 0 0
                  OS to
                                                                                    in
                                                                                    00
                                                                               vOOO
                                                                                •  *  •
                                                                               oooo
•o
 s   I
5   e
jj
I   S
-a-   o
V   g
>   id
 O   -Z

1   ^
*   ft
«
CO
•*   •* jj a
O   4J flj 4J


     *0    rl
                                                                                                        r-ti-4
                                                                                                        OO
                                                                                                        oo

                                                                                                        do
                                       O

                                       d
                                                                                                                                 O—IO
                                                                                                                            OO OOO

                                                                                                                            ddddd
               60
       CO
       o
       CM
                           CM OOO
                                                       CMOO
                                                  O O O r-t O in

                                                                                OO



                                                                                00
        CM
        O
        CM
                     60

                     i—l  0)
                     0  JJ


                     Ist
                                                                                COOO
                                                                                                 o
                                                                                                 d
                                                                                                         o
                                                                                                         d
        o
        CM
             •a
             a>   ai
             C 4)r-l
              ^i
              S
                            CO

                            I
ooo

CMOO
                                                                                                  O

                                                                                                  d
                                                                                                  o
                                                                                                   •
                                                                                                  o
                                       b
                                       o

                                       £
                                       o

                                       o
                                  OrH JJ
                                 o   eg
                                    JJ • V
                                  0) O
                                                      CO
                                                     •o
                                                     Ti
                                                     1—I
                                                      O
                                                     CO

                                                     "O.
                                                     •o
                                                      c
                                                    CO 0)
                                         01  to a  a-
                                         M  0) rl  CO
         §
         CO
                            •r-l 03 tt)
                                                           O  B -•  -
                                                           vf  9«rl>r4 _
                                                           c-ri E  e o)
                                                    ..^.^ -v

                                                    £^^^c5566,i!
                                                                                                              c «> o
                                                                                                                 JJ 4J  4J
                                                                                                              B « 03  03    01
                                                                                                              (0 i-l rH r-l 9) JJ
                                                                                                                   CD  <0 4J
                                                                                                              C J3.C X 
-------
    s
   ••sl-
 oi  to
   B  fc
 Q)  CO  01
CJOftj
          0)    U
          U  >>U
          OJr-( CO

                     e?
                    o
                         CJ* rH   VO f-H
                 OVOOOOcoa>r- u->
                                                                                          OOOOO
                                                                                          	ooooo
                                                                                                                                  I/1IOCM rH rH
                                                                                                                                  OOOOrH
                                                                                                                               oooooo

                                                                                                                               oddddd
                                                                                                                                  V  V
   o
   •C
 0)  60
 B  B
•rlM 0)
1-4  B CO

 ^g-S
                    CO
                                                                                                  \O      r-4 i-l
                                                                                                  O      r-t O
                                                                                                  O      OO

                                                                                                  o      od
                                                                                                             "1    rHi
                                                                                                             O    rHI-t O O O
                                                                                                             O    OOOOO

                                                                                                             d    odddd
            60
     f-t a)  c
   vo a 4J-H  at
   •sr^i etr-< u
   fo AJ o jd  a
         u  o
     1-fO 60

  CM  a .S.5 01
  OT< qJr-l 4J
  CO u 01 A! a
                   S
                              CM
                                                                             CMO
                                                                               •
                                                                             tv.<

                                                                             CM
        ns
        at
  2
  CO
           OB
         CO


          B?
         Q
                                                                    SCO
                                                                    O
                                                                •  •  •
                                                               •-IOO
                                                                                                 o
                                                                                                 d
                                                       o
                                                       d
0)
ti to u
0) O B
> E 01
0) ra O
CSO B
O
U

co
BJ
Q



O\OO
COv£>cx)t—i
                                                                                      OO
 o
 r-t
 CM
 00
 B
A! B
 O-H
              00-3-O
CM COO*
      CO
                                                         VO
                                                         o         oovo r^cM
                                                   OOOCOOOO\COOCO
                                                                                     voo
                                                                                     COO
                                                                                     CO
M
s
I
                          M
                          O

                         JS
                         U

                          O
                    O»-l U
                   O   C8

                       O E CO
                                              09 n
                                             •0-0
                                              o  o
                                             coco
   U

   01
   rH
   eg
rH >
                                                                                          0)

                                                                                          CO
                                                                                         J=
                                                                                         
                                    01 O
                                    0,0

                                        01  CO
                               «    0)  O J3
                               JJ    B  rf AJ
                               O    01  O  01
                               H:    NrH  o S O
                    _  _         '    S £  rl lJ U
                    E  a             oi  o  o
                    93       CO 0) Ji-rlrH
                 rHiH«-l    >JrHBOm3
                 OJBrH    0) O 0) lj H O
                'JrfOirHO>ENoT<0bQ'
                 OrH  ffl  BrH OIBrHrH XrHI.
                         •rl^JS OJXirH 01
                         N CO CU po O rH S3
                                                                                                  o ox;
                                                                                                  •u B o
   B 01  01  01
   •rl JJ  4J 4J

   CO rH rH rH 01 XJ
   i-l CO  CO CO iJ CO
   B jC J5 43 to rH
   0) 4-1 ,rH J3 C CD
01 O 01  N >-,&<    E
                                                                                                                   SS2.4J 
-------
    00
    m
    O
    so
•o


II
4J
B  <:

§  i
    u
    2
•vf

CM
• I

>



 0)
J3  CO

 cd


H  ft
CD CO

1-4 1H CuC!
ON 4J S i-l *
ON cd Cd t-l i-l
1-1 1-4 60H CO
O P
> 0
"O
0) 01
e 0)1-1
O *H 4J p*
CM JS CO B
CM s a «8
OS W
u
50

•5.C
ON rH 4J
i-i J£ cd
CM o pa
1-1
OH


•o
0) 01
O 4J >N*J
CM «i— 1 to
T-( us
H10*
0> Ml
B C
•J-1 •!-) (U
\O rH C EQ
o to to c

O i-i JJ cd cd
o cd "O u ><
CD.O a co B HE
£C3 !Ti W §™^ E 01 CO fl)
CuCX32!V4C^> EBiHEEQJ cdCD
"e">'l!co'o2Scxo'cd s'lj
•H Cd CD >. >fr< r-ljSOBVJCd^lJSOrJaiCd'r';
CO
m .3- m
VOrH CM T-l f^-
OO O . O PO
ooooo oo oo •
ooooo oo oo
V -

co mo o oo m o ooo
00000,000000000000000 ooo
V V




O CO O
OTHO
o
s

CM ao r~m ON mm
\o o o po r-i oo
CMOOOOOOOOOOOOOOOOOOOOOOP
CMOOOOOOOOOOOOOOOOOOOOOOO
V V V

o
r-4 V V V

cMr-400 PO cMmcMoo m 1-11-4 co
h»ooo o ooi^-ff o mm o
3OVDO-*OOO OO OO OOOOO OOOOOOO
•^ V V V.

m
ONOO
r~-oo
^H


B 01 01 0) 0)
0) 1-1 4J 4J AJ 4J 0>
B 0) B « « rt OJ 0) B
cd a) T> cdi-4i-iT-ii-ia)4u CD a>
j30) B 1-1 r-icdcdcdcd*jcd 1-4 B
4J B 0) V-t B JO* £* *£- ^2 cd i— 4 ^ Q)
1— 1 CDCd 3 O 0) 4J JJ 4J 4J i— 1 Cd JC T-^
cd w o x: TH rH i^ijsjSJS'S^ AJ ^>
JJ B^J-1 OCU.B CXCU CUPn P-i JS 4J 0) 0) < «C
O CDOO) JJBUO)iHr-4r-4 4J JS CO U
H Ni-IOBOO) B-DX >%r-4 i-l JS P* CD 0) U 0)
B£hh^NO)cuoa)(o x^cb B i-i o o
BE " CDCJOOAJCBl— ICQJ3B4J4J l-40).£l-4 t)
33 CO 0) rO i-l i— 1 tM*HO}QJcdOr>%0)dOr«H^irJUtCQJO
^•^ ^i— !CO^lj3OC^i-4»CI-l43^PQCD >>*C cd B O B i— 1
CJ r—t 0} O 0) M H O M i-l r— 1 ^> AJ 4J JJ r-^ f 1 J^ U V Cd Cd Q) •£•
0) r-4 CJ&BNO' CdOQ ^*J* «d iH W ^^ 2UJcD4-BV)?O
1-4CH C ri 01 Bl- Xi-U OuZ ' 4J « 1 0)SJ->OIUr-li-<
fli .C *r4 *»^ jC 0) >£ '""I QJ .C ^0 W fl) QJ ' P^ <3 "p4 »H *»~^ »r^ C! <£ QJ O ti
                                                                165

-------
              CO
              10
              CM
                 ta a
                (A u
                                  OOOO
                                       POO

                                         oo
                                         o
                                         m
                                         oo
                                         CM
                                         vo
                                                   PO
                                              OOOs
                                              ooio
                                                             ovo r^oo co
                                                        VO   CM   PO
             CM
             IO
             CN
                0 Q)
                OS 4J
                                 ooo
                                                                CM
                                                        OOOOVOVO
                                         O     00
                                          • OO CMVD
                                         o  •  •  •  •    .  ,  .  .  .
                                  ^.-    JOOOOrH   OO-
                                               • OOCM 1O
                                              o
                                                          vOvO
                                                        O f»- PO CO OO
                                              VOPO

                                              1OVO
I
m
21
o
             CM
                     « 0)
                    OS U
                                 OOCMO
                                      rHO
                                        o
                                      -  o
                                                       VO
                                             o o o o m
                                           §">O OO
                                           C
                                                CM
                                                       CMCMOOtO
                                                       00
*   3
                                OOrHO   OOOOO   OOOO CM OO

                                             OlOOOO   ••» O vo O O
                                             Of-                CM
                                     COOO
                                        00
                                                                                                                           CMCM   CM V
       to
       rH
       CM
                 •O
                  0)    Q)
                  C fl) r-l
                 *r4 U  Q
                 J5 ra  ff
                  9 a  w
                  OS=w
                    CO
                    B
            OJ
            o
            CM
                                     CMCM
      g
      M
      S
           K>
                                               a>
                                             BtJ
                                             O-rl
                                    0°
                                        ,J O
                                        q) CO

                                          •o
                                  O    O-D

                          S3 33 U to    BO)
                           CX O* 9 0) CO  B CX
                                JJ (4 0)  CO tQ
                           m a 
                                                                                       .CO)    B   i-l
                                                                                       •u B  ' 0)    b
                                                                                       «) a)    3    o
                                                                                     0) O f   rH   rH
                                                                                     B M 4J.   o OJ.C
                                                                                     OOO)   JJ C O \u -n r-f rH      OJ
                                                                                     NrHOBOtt)    CTJX  >,rHrHj;i
                                                                                     B^!Vlr4UNO)a)OO)NX XCU
                                                                                     0) O O.O 4J C  BrH COX!  B 4J U   r
 c o>  o) a)  at
•rj 4J  4J U U
 B cd  ccJ c[j  m

rH CD  cd W  « U '
 C J3 J3 J3 J3 edr
 01 4J  4J 4J tlrH
£,&£,£.jz eg.
                    0) 0)
                    c o
                                     -..-c'seS      3'5'BS   S§8
                                     OrHrH«H Q) O O O4C*t7 6>0«M 0) I—I CJ > ta O •
                                    5"*JtJOJiJiJCUpM C? O rH Cd B rH B rH rH
                                    _innnt.-.«-...._.  -airJ^^ialj-rHu,
                                                                  ~   10 CO (0 OrH -S
                                                                                            oo
                                                                                          X r-l  I
                                                                                                                            B O
                                                                                                                            « «
                                                                                                       .
                                                                                                    ) co  i CM
                                                                                                                               
-------
      4J  tO
       O  B
r-i  i  cd i-<
.-I  C •U i-l
CM  o  c  o
   s  o  o:»
      00
              O OenOO O

              in vo r-oo o
       00    E:
       C 4J Cd
O T3i-< B O
i-l r-l f< 41 -rl
CS Qr-t &, M
    O O CO ,fi
              00
                              o
                              o
                              o
                              u-1
                              en
                              oo
                                                 OOOOOO
                                                 O-*
                                                            OO OO i-l «-H en tri O
                                                                        1-400
                                                                           CM
 CM
 CM
          i-l  0)
           cd  w
                                  u-i
                                  O       1-1
                         u-i VJB O O O O en
               i/i i/i m O O en O       i-*
      • •o
        0)
        e
       •
       .QMS
        B
o
CM     B  cd cd
       OSto
                                                                                                                                    OOO
               CM \Oi-l
                     CM
 CM
 CM
 60
 C
•rl  ^
•-<  41
 C8  4J
  uiui

                               Sen
                                CM
                               OOO
  O
  CM
•G
 4)     4)
 B  4)i-l
i-l  4J  g
ft  to  S
 S  cd  cd
 OSCO
                CM en CM
                      CM
                                             00
                                          oen
                                         -*o
                                         en
OOOI>>
         ey>
                                                                                                                   41 41 41
                                                                                                                ., .  4J 4J 4J
                                                                                                          41    S  cd cd cd 41

                                                                                                                i-i  cd cd
                                                                                                          p    B  f J5^_.
                                                                                                          O    41  4J 4J JJ Cd
                                                                                                                .£  <
   H

   g
   0,



   CO
                                                                                                                                                4)

                                                                                                                                                41
                                                                                                                                                      41
                                                                                                                                                      B
                                                                                                                                                      4)
                                                                                                                                               4J     >>
                                                                                                                                            4) 41    A
                                                                                                                                            BO    -U
                                                                                                                                         41 41 P     4)
                                                                                                                                -- , .    B (J O     O
                                                                                                                 _  „ .	B4Ji-l4)X!i-l     H
                                                                                                                 (DCU«O^Q)O>->OtJJ2Q)O
                                                                                                                        --  — -— — ^ — (jBr-^
                                                                                                                                      _ .. -. Cd  41 JC
                                                                                                                             „ .	4)4=SI-i30
                                                                                                                          „ I  U I  S U 41 4Jr-l i-l
                                                                                                                          l-NS^-ri e.,e ai  o^
                                                                             167

-------
       •O    JJ
       0) *O B
       B  0) 0)
       •n jj 3
       43  <3rH
       B  «<4H
       O  U*W
       OH W
                                                                                                                 if} ir,      o
                                                                                                                 o o      o
                                                                                                          o    oo oooo

                                                                                                          d    do dddd
   jj

   l!
 ag
3ti
 a o
    u-i
    W
        js a>
        Opj
                     •3-eo
                                   
                   en co

                   invo
                                                                                                          O
                                                                                                          v
                                                                                                                  O
                                                                                                        O\ ON     O
                                                                                                      oo oooo

                                                                                                      do dddd
                GJ
               O
                    oo   ooon
                            oocoo
                                CM
                                                                                                              oo oooo
                                                                                                                CO CO
                                                                                                                CM CM
o
sr
      0)
      O    M
      MrH 0)
      ooo
                   OUtCOOOOcOM

                   vovocMoodod
                              M
                              O
                                          CO
                                        B'O
                                        OfH
2
                             o
                       o°-3u


                   KBrill
                   Cud. 3   <
                               o) co
                               (-1 O

                              o w
                                 •D
                               O 13
                              -rl e
                            ra B a;
                            3 OS Cu
                                                   JJ

                                                   01
rH >
 CD (8
                                                                        (d
                                                                        JJ
                                                                       5
   u
   C
   a
  43 01
  4J B
   0) ffl
01  O43
a  M JJ
01  O 01
tO f-H O
                                                                                      0)
          B 0) II) 0) 0)
          •rl JJ JJ JJ JJ
     0)   S « « ed c8    01
     •O   KtrHrHrHrHCUJJ




rH


JJ B D 01 ^ r-Tr^T     JJ 43
O 01 .. B -0 X !>»rH rH 43 (rl 0)
                                                                                                            (SrH
                                                                                                0) JJ 4J JJ 4J i-f  ffl
                                                                           B43.fi»J>JN010iOdJ  N'>,'^E
   0)
   01
  rH

  I
01  01
B  O
01  W
 0)

 0)
rH

£
                                                      168

-------
•o
0)
B
ft
U
1
s^
in


0)
1-4
a


i
§
u
z
H
J
PM

i'
SH


in
I-l
CM






S
CM


•o
ID e
B 0) CO
•f"t AJ Q)
43 CO M
5 **
U




60
5.
i—* CO
23


CM
I





CM
*


©©CO ©©©©CM
IAI*^** ©ino©o
CO OOCM
oom
I-HCM





• CO
r-iOOOOi~iOOOOOO
CO CO I~»VO
l-<


CO
in oovoco f* co
or-
CM
                CM
                     OO©
                                  ©OOCMVO
        CM.
OOOOVOVO
r^.i»-o©   ©»©©!-<
     ^•O   moo      i-«
        \o   coin
        00   CO-*
        CM   vo
I».CO
     ^-
     OO
                                                                            ©0©©©©©©^©©©°©
                  OO rH
tM

CM
I


© ©r»©
o\ c\ so ©
CO©
o
o
!-<
00 rH
OO-*i-l©
§OOO©
VO
covO.
1-4
O^ i-*-*
©CM O-*CM
1-4 00
i-l i-l

                                                                     o©
                                                                                                     e  CD o  o CD
                                                                                                    ^-1 4J 4J  4J 4J
                                                                                                     S  0) «  W «

                                                                                                               
-------
                   I?
                   o
                         OO
                          •  •
                         in in
    OOOOCM
                                                                                  O\   OOOOCM
                                                                               O r-» O O CM i-H O
                                                                                              333
                                                                                              P p p         f> CJ\
                                                                                              COO
                                                                                     O.CJS    OO
                                       o
                                       I-.
                                       CM
                                                                                               ••
                                                              OOOOO   Or-HOOi-lCMO
                                                              U1\D            SO
                                                              00-*
 CM
 CM
          to
          0)     E

I    I
CM
CM
          60
         f-4 0)

          Si JJ
                                                                                                                                OOOOOOOOQO
*    (3
61    E
          60
                                      OOOO1OOOOO»HOOOCMCOO
CO
o
CM
                        to

                       I-)  fl)
                       r-l  CO
                       X  C
         PW
                 CM


                 I
                                     CM mo
                                           CM
                                                                                                                                  V    V    V  V
                                   O
                             Ol-H U
                            o   B
                                U  . fl)
                             0) O C 01
                       S3 ffi MH B «
                        (X 0.3    < QI
                       a B a a)
                       3 E
                       e m
                       -»r! CKis e     o
                       e x a ca 8)1-1
                          e o
                                               Oi-l
   M O
   eg co
  o
     •O

  i-l *C
01 B 0)
900.
M 60 co
                                                                            0)
                                                                           i-l


                                                                            I
                                                                                                   eg
                                                      "O O H  3  B
                                                      •rl SlOU)  Q

                                                          CO i-l i-l >r4
                                                                      O  3
         01
         CO
         0)
U        B<-<
Oi        eg  01    d)
a. B •o  toj B
a.oe  a>
                                                 i-l 4J 4J  4J
                                                 E eg eg  eg
                                                 eg i—I r-f r-4 Ot
                                                 i-i eg eg  eo 4J

                                                 01 4J u  u i-<
                                                  	eg
                                                          01
                                                          B
                                                          01
                                                                  MiJEJSNCOQHeOOi-*
                             0) 1-1 iH rH    U

         BJ=WU    N    B'D^  ^7' -13 W
    »    0>CJOO.L)BBi-
   eooi^>>Hi-''Wi-40ia)ego>>oi
iJi-i  B  O^J3 O CJZr-if  UJ2£>
   O(llUHO)-li-li-IX4J4JJJr-l    _„
   "'NO'  eg o a >*f £ -H W  S>,S u J3
      Ct—ii—i >»J
   o
                                                                            I  OrH  O
                                                                            i O  >>cfl
                                                                            c  ' JS  ti
•UJB
B O
eg eg
B M
  jd
  4J
   01
   o
   k

-------



00
o
CM



0)
4J

CO 0)
CO
CO
6*


CM
cd
O




r*. t*» o
• • •
VOVOO
CM



                                                                                                                                  1O1O     O
                                                                                                                                  oo     o
                                                                                                                          O   OOOOOO

                                                                                                                          O   OOOOOO
                                                                                                                                  v v   I-H v
       O
       CM
                                           moo            r~eMm«3;   oo
                                         O.CM cooOOOOOrHrHOCOO

                                         dddrHinooooooooo
                                                                                      oo
                                                                                                                                    OOOOOO
                                                                                                                                      •  •••••
                                                                                                                                    OOOOOO
     •O    4J
      wo e
      B CD 0)
O   tH U 3
C5   .O (C f^
•&    e o)
rH M 0 3
M-IWH tH"O
w-i .So)
W O D^
CM
a
GO CO
inOvOOOOcovO
 p o a o
 -* rH JJ O 3
 CM IM    rt ti
   B   .CO)
ON
rH
CO
              a) o W  0 -rl
                                 m-* m

                                 CM in oo
                                         OO
                                  oooo

                                  in 060^
                                                            t»-
                                                 ooooo
                                              mo
                                              CO
                                          ID VOOO O
                                          ON 00
                                                                            «o o
                                                                                                                                             o
                                                                                                                                             o
                                                                                                                                 OOOOOO

                                                                                                                                 ddddoo
                                                                                                                                    tno
                                                                                                                            00 CO    OO
                                                                                                                         O i-t iH OO O

                                                                                                                         ddddod

ON
rH
CM
4J
0)*rl 0)
3 O g
M-l O*H
B •<-> Jd
M CO
CM
CO
Q
OO OOO-*
mcM OOOO
CO
r-
CM
O OOOO
r-~ CMO o o
co-o-
rH rH
vooomoo
VO rH rH CM O
rHOCMOO
                                                                                                                            o
                                                                                                                            o
                                                                                                                                                   o
                                                                                                                                         mtn      o
                                                                                                                                      ooo ooooo
                                                                                                                                       •  •••••
                                                                                                                                      OOOOOO
               0)
               o>-i
         rH    3 0) JJ
               OS* «
                             \OvOi-lOOOOO<-l
          g

          I
          PH

          CO
                                                                           171

-------
       0
      01
ss-a
   m a
   s> w
                       OOvO
                             cot
                              • oo
                               o
                               CM
                                        O
                                        o\
                                             ooo
                                                                                                            oo

                                                                                                            00
                                                                                                                   o
                                                                                                                     O

                                                                                                                     O
                                                                                                                                   CMtM o
CM
O
CM
          to
Jd C
 O-rJ
                 CO
                                                                                                        csooooo    o   oooooo
                                                                             £0    ooo'oo'd   ddddod    d   dddddd
CM
                      oooo
                r-.i-.coo
                     coo
o

o

00
CM
VO
                                             OO«A
                                                        VD   CM
                                                                               \o
                                                                            OCM
                                                                              •  •
                                                                            OO
                                                                            CM
                                                                            CM
                                                                                O    O
                                                                                O    O
                                                                           ooooo

                                                                           ddddd
                                                                                V    V
          S) g)
            CO
            £
                      O OOOO

                          •*r>.O
                           CO 1-1
                                        o
                                         •
                                        o
                                       in
                                       CM
                                                  o-
                                            ooo
                                                                oo
                                                          -a-    i-<
                                   OOO    U1OCOOO
                                                                    •»            ooo      or-                    oo
                                                                    ^O    OOOOO   OOOOOCNOOOrtOOOOOO

                                                                    vod    ddddd   dddinddddd dd-Jr-Iddd
                                                                                                      CM                     CM CM v i-< v
2

g
5
CO
                  0°
                      r-l
                                U O
                                a u
                                o
                                   •o
                                o -o
                                •rl B
                             B c a)
                          CO w C(] Qu
                          01 M 60 CO I
              4J


              CD
             i-l



             I
                                                  S  B
                                                       a. c-o
                                                          4) BiH    S
                                                        W 
                                                          UrH CO Cf-l
   w  '

   co  :
  £  0)

   cu  «
a>  ox:
B  M XJ
a>  o  a)
Nr-l  O S
                                                                             01 u  o

                                                                            i o
                                                                                                                C Q)  0)  0)   h
Vl  O
                                                                                                                                  cd B  O
                                                                                                                                     01
                                                                                                                                     B
                                                                                                                                     0)
4J
01

2
                                                                 172

-------
4J
00 B
BUS)
O-Oi-l B O
rH rH i-H a> -iH
CM O rH O, (H
u OKI .n
erf 3
•J

CO
>1
td
Q



OOvo
in m m
CM



                                          O
                                          O
                                          CO
                                                 O
                                                 in
                                                 cr>
                                                 rH
                                                 VO
                                                      ooo
           CM

           CM
                   5u
                   rH  4)
                   CS  AJ
                   0)  CO
                   B  S
                                                                                                      ooooooooooo
                                                                                                                  oooooo
    VO
    o-
    \o
m
o
CM
                      0)
                •o
                 a)
                 e
                IH u &
                js co a
                 E cd «
                 OSco
                               CM tJIVO
•o

 I
 c
1-1
 u

 §
V.
     IS
vO
CM
CM
in   o
CM   Z
 •    H
>   J
     P-I
     o

     !H
                   OS
                   r-< a)
                    (0 4J
                    £03

                    C
                   ^ C
                    0-rl
co



o*
                                                                                                                       OOO O
            CO
            O
            CM
                                            C5C5
                                                                                                                   OO OO OO
             o
             CM
                  •o
                  Q)    a>
                  C  a) rH
                  •rl  U ft

                  iS§
                  o  » en
                  o
                                                                                                                        oooo
                                                                                                                      v v
             S



             Cu


             CO
                                                                       173

-------
    4> K
    <-« O    JiJ
    •dxrl  &.E

 o> a B  Ur-<
                               CO


                               ,
                                                                                                                                              oooooo
                                                                                                                                                 V V       V
                 •u    E  O
                 c    g *H
                 a» e—< u
              c> g o H  o
              -*r-i M o  g
              COU-HM Jj-o
                 IM   JT  ffl
                 w   o pi
                      CMOO        COO\      OOOOO VOCMCOin      OO
                       •••          ••        •••••••••       ,,
                      cMcot^        OCM      oo r^o oo 1-100 CM      oo
                           •-*                              BNOI  eoo
                                                                                                                            r-iaaa«u«.      r-<
                                                                                                                                             .Cl    BO     >
                                                                                                                                             K  01 5 ti    0)
                                                                                                                                                C S 0    0
                                                                                                                                                a B o  B .
                                                                             174

-------
                                  §oooo
                                  Oomo
                                                ON

                                                COON
                                                CMOO rH
                                                             O-vO


                                                             ON ON
                               vO irt i-l
                               eo<-i
                                        ON CO
                                §
                                in
           o
           aj
           e
                  •O
                                     o

                                OOON
                           OOO-
                           1-1 CO
CM
 I
•8
H
1-1
 CO
1-1
 (J
 0)
 4J
I

 co
 (0


 o>
 u
 M

 §,
 CO
 i-l
 es


 «l
•O
 O
£

 o

3
            o
           u
            g,

            u
                   o-
                   VD
                   O
                   VD
                                      ooo-
                                ITli-l
                                i>-
                                O-
                                CM
                                        -*oo
                      I--CM
                                 ooooooooo-*
                                       1^^f>    O r*
                                         oo         1-1
                    c
                    9
                      OOv&O O
                            oo 
-------

-------
                            SECTION VI

                SELECTION OF POLLUTANT PARAMETERS
The Agency has studied copper  forming wastewaters to determine
the presence  or  absence  of  toxic,  conventional  and  selected non-
conventional  pollutants.  The  toxic pollutants  and  nonconven-
tional pollutants  are subject  to BAT effluent limitations  and new
source and pretreatment  standards.  Conventional pollutants are
considered in establishing  BPT, BCT, and NSPS.

One hundred and  twenty-nine toxic  pollutants  (known as  the 129
priority  pollutants) were studied  pursuant  to the requirements of
the Clean Water  Act  of 1977 (CWA).  These pollutant parameters,
which are listed in  Table V-l  (p.79  ), are members of  the 65
pollutants and classes of toxic pollutants  referred to  as  Table  1
in Section 307(a)(1) of  the CWA.

From  the  original  list of 129  pollutants, three pollutants have
been  deleted  in  two  separate amendments to  40 CFR Subchapter N,
Part  401. Dichlorodifluoromethane and trichlorofluoromethane
were  deleted  first (46 FR 2266, January 8,  1981)  followed  by the
deletion  of bis-(chloromethyl) ether  (46 FR 10723,  February 4,
1981).  The Agency has concluded  that  deleting  these  compounds
will  not  compromise  adequate control over their discharge  into
the  aquatic environment  and that  no  adverse effects on  the
aquatic environment  or on human health will occur as  a  result of
deleting  them from the list of toxic pollutants.

Past  studies  by  EPA  and  others have  identified  many nontoxic pol-
 lutant  parameters  useful in characterizing  industrial^wastewaters
and  in evaluating  treatment process  removal efficiencies.   Cer-
tain  of these and  other  parameters may also be  selected as
reliable  indicators  of  the  presence  of specific toxic pollutants.
For  these reasons, a number of nontoxic pollutants  were also
 studied for  the  Copper Forming Category.

Congress  has  defined the criteria for the selection of conven-
tional pollutants  (43 FR 32857 January 11,  1980).   These criteria
 are:

 1.  Generally those pollutants that are  naturally occurring,
 biodegradable; oxygen-demanding  materials,  and  solids that have
 characteristics  similar  to naturally occurring, biodegradable
 substances;  or,

 2.  Include  those clases of pollutants that traditionally have,
 been the primary focus  of wastewater control.
                                177

-------
 The conventional pollutants considered (total suspended solids
 oil and grease,  and pH) traditionally have been studied to
 characterize industrial wastewaters.   These parameters are
 especially useful in evaluating the effectiveness of wastewater
 treatment processes.

 Several nonconventional pollutants were considered.   These
 included phenols (total),  fluorides,  phosphorus,  iron, manganese
 and total organic carbon (TOG).   None of these pollutants  were
 selected for regulation in establishing effluent  limitations
 guidelines for the Copper  Forming Category.

 RATIONALE FOR SELECTION OF POLLUTANT  PARAMETERS

 The Settlement Agreement in Natural Resources Defense Council,
 Inc-  vs.  Train,  8 ERG 2120 (D.D.C.  1976),  modified 12ERG 1833
 (D.D.C.  1979), which  precedes  the CVA,  provides for  the exclusion
 of  particular pollutants,  categories,  and  subcategories.

 Pollutants that  were  never detected,  and that were never found
 above their analytical quantification level,  were eliminated  from
 consideration.   The analytical  quantification level  for a  pollu-
 tant  is  the minimum concentration at  which that pollutant  can be
 reliably measured.  For the toxic pollutants  in this  study, the
 analytical quantification  levels  are:   0.005  mg/1 for pesticides,
 PCB s,  chromium,  and  nickel; 0.010  mg/1 for the remaining  toxic
 organic  pollutants and cyanide,  arsenic,   beryllium,  and sele-
 nium;  10  million fibers per liter (10 MFL)  for  asbestos; 0.020
 mg/1  for lead and silver;  0.009 mg/1  for copper;  0.002 mg/1 for
 cadmium;  and 0.0001 mg/1 for mercury.

 The pesticide TCDD (2,3,7,8-tetrachloridibenzo-p-dioxin) was  not
 analyzed  for because  a standard  sample  was unavailable to  the
 analytical  laboratories.   Samples collected by  the Agency's con-
 tractor were not  analyzed  for asbestos.  Data on  asbestos  content
 are available for  a very small number of samples  relevant  to  this
 study  as  a result  of  the first phase  of a  screening program for
 asbestos  in  a wide range of industrial  categories.  Of these
 samples,  only a  few appear to contain asbestos  at  analytically
 significant  levels.

Pollutants which were  detected below levels considered  achievable
by  specific  available  treatment methods were  also  eliminated  from
 further consideration.   For  the toxic metals, the  chemical pre-
 cipitation,  sedimentation,   and filtration technology  treatability
values, which are presented  in Section VII were used.  For the
toxic organic pollutants detected above their analytical quanti-
fication  level, treatability levels for activated  carbon tech-
nology were used.  These treatability values  represent  the most
                               178

-------
stringent treatment options considered for pollutant removal.
This allows for the most conservative pollutant exclusion based
on pollutants detected below treatable levels.

DESCRIPTION OF POLLUTANT PARAMETERS

The following discussion addresses the pollutant parameters
detected above their analytical quantification level in any
sample of copper forming wastewater.  The description of each
pollutant provides the following information:  the  source of the
pollutant; whether it is a naturally occuring element, processed
metal, or mamifactured compound; general physical properties and
the form of the pollutant; toxic effects of  the pollutant in
humans and other animals; and behavior of the pollutant in a POTW
at concentrations that might be expected from industrial
discharges.

Benzene  (4).  Benzene  (CgHg) is a clear, colorless  liquid
obtained~mainly from petroleum  feedstocks by several different
processes.  Some is recovered from light oil obtained  from coal
carbonization gases.   It boils  at 80 G and has a vapor pressure
of 100 mm Hg at 26°C.  It is slightly soluble in water  (1.8  g/1
at 25°C) and it dissolves in hydrocarbon solvents.  Annual U.S.
production is three to four million tons.

Most of  the benzene used in the U.S. goes  into chemical manufac-
ture.  About half of that is converted to  ethylbenzene which is
used to  make styrene.  Some benzene is used  in motor  fuels.

Benzene  is harmful to human health according to numerous pub-
lished  studies.  Most  studies relate effects of  inhaled benzene
vapors.  These effects include  nausea, loss  of muscle  coordina-
tion, and  excitement,  followed  by  depression and  coma.   Death is
usually  the result of  respiratory  or cardiac failure.   Two  spe-
cific blood disorders  are related  to benzene exposure.   One  of
"these,  acute myelogenous  leukemia, represents  a  carcinogenic
effect  of  benzene.  However, most  human  exposure  data is  based on
exposure in occupational  settings  and benzene  carcinogenisis is
not  considered  to be  firmly established.

Oral  administration  of benzene  to  laboratory animals produced
 leukopenia, a reduction  in  number  of  leukocytes  in the blood.
 Subcutaneous  injection of benzene-oil  solutions  has produced sug-
 gestive, but not  conclusive,  evidence  of benzene carcinogenisis.

 Benzene demonstrated  teratogenic effects in laboratory animals,
 and mutagenic  effects  in humans and other animals.

 For maximum protection of human health from the potential carcin-
 ogenic  effects  of exposure  to benzene through ingestion of water
                                179

-------
                                            E
 and contaminated aquatic organisms, the ambient water concentra-
 tion is zero.   Concentrations of benzene estimated to result in
 additional lifetime cancer risk at levels of 10~7, 10"", and
 10~5 are 0.00015 mg/1, 0.0015 mg/1, and 0.015 mg/1,
 respectively.                               !

 Some studies have been reported regarding the behavior of benzene
 in a POTW.  Biochemical oxidation of benzene under laboratory
 conditions,  at concentrations of 3 to 10 mg/1, produced 24, 27,
 24,  and 20 percent degradation in 5, 10, 15, and 20 days, respec-
 tively, using unacclimated seed cultures in fresh water.  Degra-
 dation of 58,  67, 76,  and 80 percent was produced in the same
 time periods using acclimated seed cultures.  Other studies pro-
 duced similar  results.  Based on these data and general conclu-
 sions relating molecular structure to biochemical oxidation, it
 is expected  that biological treatment in a POTW will remove ben-
 zene readily from the  water.   Other reports indicate that most
 benzene entering a POTW is removed to the sludge and that influ-
 ent ^concentrations of  1 g/1 inhibit sludge digestion.   There is
 no information about possible effects of benzene on crops grown
 in soils amended with  sludge containing benzene.

 Carbon Tetrachloride  (6).   Carbon tetrachloride (CCl^.),  also
 called tetrachloromethane, is a colorless liquid produced primar-
 ily  by the chlorination of hydrocarbons - particularly methane.
 Carbon tetrachloride boils at 77°C and has a vapor pressure of 90
 mmoHg at 20  C.   It is  slightly soluble in water (0.8 gm/1 at
 25 C;  and  soluble in many  organic solvents.   Approximately
 one-third  of a million tons is produced annually in the  U.S.
                                            i
 Carbon tetrachloride,  which was displaced by perchloroethylene as
 a  dry  cleaning  agent in the 1930's,  is used principally  as  an
 intermediate for production of chlorofluoromethanes for  refriger-
 ants,  aerosols,  and blowing agents.   It is also used as  a grain
 fumigant.

 Carbon tetrachloride produces a variety of toxic effects  in
humans.  Ingestion of  relatively large quantities  - greater than
 five grams - has  frequently proved fatal.   Symptoms are  burning
 sensation  in the  mouth, esophagus,  and stomach,  followed  by
 abdominal  pains,  nausea, diarrhea,  dizziness,  abnormal pulse,  and
 coma.  When  death does  not  occur immediately,  liver and kidney
 damage  are usually found.   Symptoms  of chronic  poisoning  are not
as well  defined.   General  fatigue, headache,  and  anxiety have
been observed, accompanied  by digestive tract  and  kidney  dis-
comfort  or pain.

Data concerning teratogenicity  and mutagenicity  of carbon tetra-
chloride are scarce and inconclusive.   However,  carbon tetrachlo-
ride has been demonstrated  to be  carcinogenic  in laboratory
animals.  The liver was the target organ.
                               180

-------
For maximum protection of human health from the potential carcin-
ogenic effects of exposure to carbon tetrachloride through inges-
tion of water and contaminated aquatic organisms, the ambient
water concentration of zero.  Concentrations of carbon tetrachlo-
ride estimated to result in additional lifetime cancer risk at
risk levels of 10'7, 10'6, and 10'5 are 0.000026 mg/1,
0.00026 mg/lj, and 0.0026 mg/1, respectively.

Data on the behavior of carbon tetrachloride in a POTW are not
available.  Many of the toxic organic pollutants have been inves-
tigated, at least in laboratory-scale studies, at concentrations
higher than those expected to be found in most municipal waste-
waters.  General observations have been developed relating
molecular structure to ease of degradation for all of the toxic
organic pollxitants.  The conclusion reached by study of the
limited data is that biological treatment produces a moderate
degree of removal of carbon tetrachloride in a POTW.  No informa-
tion was found regarding the possible interference of carbon
tetrachloride with treatment processes.  Based on the water
solubility of carbon tetrachloride, and the vapor pressure of
this compound, it is expected that some of the undegraded carbon
tetrachloride will pass through to the POTW effluent and some
will be volatilized in aerobic processes .
Chlorobenzene (7).  Chlorobenzene
                ~
                  .                           also called mono -
 chlorobenzene Ts~a  clear,  colorless,  liquid manufactured by the
 liquid  phase chlorination  of benzene  over a catalyst. o It boils
 at  132°C  and has  a  vapor pressure of  12.5 mm Hg at 25  C.  It is
 almost  insoluble  in water  (0.5 g/1 at 30 C) , but dissolves in
 hydrocarbon solvents.   U.S.  annual production is near  150,000
 tons .

 Principal uses  of chlorobenzene are as a solvent and as an inter-
 mediate for dyes  and pesticides.   Formerly it was used as an
 intermediate  for  DDT production,  but  elimination of production of
 that  compound reduced annual U.S. production requirements for
 chlorobenzene by  half.

 Data  on the  threat to human health posed by chlorobenzene are
 limited in number.   Laboratory animals, administered large doses
 of chlorobenzene  subcutaneously,  died as a result of central
 nervous system  depression.  At slightly lower dose rates, animals
 died  of liver  or  kidney damage.  Metabolic disturbances occurred
 also.   At even  lower dose rates of orally administered chloroben-
 zene  similar  effects were observed, but some animals survived
 longer than  at  higher dose rates.  No studies have been reported
 regarding evaluation of the teratogenic, mutagenic, or carcino-
 genic potential of chlorobenzene.
                                181

-------
 For  the  prevention of adverse effects due to the organoleptic
 properties  of chlorobenzene in water the recommended criterion is
 0.020 mg/1.

 Only limited  data are available on which to base cone ITIS ions
 about the behavior of chlorobenzene in a POTW.   Laboratory
 studies  of  the biochemical oxidation of chlorobenzene have been
 carried  out at concentrations greater than those expected to
 normally be present in POTW influent.  Results  showed the extent
 of degradation to be 25,  28,  and 44 percent after 5, 10, and 20
 days, respectively.   In another, similar study  using a phenol-
 adapted  culture 4 percent degradation was observed after 3 hours
 with a solution containing 80 mg/1.  On the basis of these
 results  and general  conclusions about the relationship of molec-
 ular structure to biochemical oxidation, it is  concluded that
 chlorobenzene remaining intact is  expected to volatilize from the
 POTW in  aeration processes.   The estimated half-life of chloro-
 benzene  in water based on water solubility, vapor pressure and
 molecular weight is  5.8 hours.
                                            i
 1,1,1-Trichloroethane (11).   1,1,1-Trichloroethane is one of the
 two  possible  trichlorethanes.   It  is manufactured by hydrochlori-
 nating vinyl  chloride to  1,1-dichloroethane which is then chlori-
 nated to the  desired product.   1,1,1-Trichlproethane is a liquid
 at room  temperature  with  a vapor pressure of 96 mm Hg at 20°C and
 a boiling point of 74°C.   Its  formula is CCl^CR^.   It is
 slightly soluble in  water (0.48 g/1) and is very soluble in
 organic  solvents.  U.S. annual production is  greater than one-
 third of a million tons.

 1,1,1-Trichloroethane is  used  as an industrial  solvent and
 degreasing agent.

 Most  human toxicity  data  for  1,1,1-trichloroethane relates to
 inhalation and  dermal exposure routes.   Limited data are avail-
 able  for determining toxicity  of ingested 1,1,1-trichloroethane,
 and  those data  are all  for  the compound itself,  not solutions in
water.   No data are  available  regarding its toxicity to fish and
 aquatic  organisms.   For the protection  of human health from the
 toxic properties  of  1,1,1-trichloroethane ingested through the
 comsumption of  water and  fish,  the  ambient water criterion is
 15.7  mg/1.   The  criterion of based  on bioassays  for possible
 carcinogenicity.                            :

No detailed study  of 1,1,1-trichloroethane behavior in a POTW is
available.   However,  it has been demonstrated that none of the
toxic organic pollutants  of this type can be broken down by bio-
 logical  treatment  processes as  readily  as  fatty  acids,  carbohy-
drates ,  or proteins.
                               182

-------
Biochemical oxidation of many of the toxic organic pollutants has
been investigated, at least in laboratory scale studies, at con-
centrations higher than commonly expected in municipal waste-
water.  General observations relating molecular structure  to ease
of degradation have been developed for all of these pollutants.
The conclusion reached by study of the limited data is that^
biological treatment produces a moderate degree of degradation  of
1 1 1-trichloroethane.  No evidence is available  for  drawing con-
clusions about: its possible toxic or inhibitory effect on  POTW
operation.  However, for degradation to occur, a  fairly  constant
input of the compound would be necessary.

Its water soltibility would allow 1,1,1-trichloroethane,  present
in the influent and not biodegradable, to pass through a POTW
into the effluent.  One factor which has received some attention,
but no detailed study, is the volatilization of the lower  molecu-
lar weight organics from a POTW.  If 1,1,1-trichloroethane is not
biodegraded, it will volatilize during aeration processes  in the
POTW.

Chloroform  (23).   Chloroform  also called trichloromethane, is  a
colorless liquid  manufactured commercially by  chlorination of
methane.  Careful control of  conditions maximizes chloroform pro-
duction, but other products must be  separated.  Chloroform boils
at 61°C and has a vapor pressure of  200 mm Hg  at  25 C.   It is
slightly  soluble  in water  (8.22 g/1  at  20 C)  and  readily soluble
in organic  solvents.

Chloroform  is  used as  a  solvent and  to  manufacture refrigerants,
Pharmaceuticals,  plastics,  and  anesthetics.   It  is seldom used  as
an anesthetic.

Toxic effects  of  chloroform on  humans  include central nervous
system depression, gastrointestinal  irritation,  liver and kidney
damage and  possible  cardiac sensitization  to adrenalin.   Carcino-
genicity  has been demonstrated  for  chloroform on  laboratory
animals.

For  the maximum protection of human health from the potential^
carcinogenic  effects  of  exposure  to chloroform through ingestion
of water  and  contaminated aquatic  organisms, the ambient water
concentration  is  zero.   Concentrations  of chloroform estimated to
result in additional lifetime cancer risks  at the levels of
 10'7, 10'6,  and 10~5 were 0.000021 mg/1,  0.00021 mg/1, and
 0.0021 mg/1,  respectively.

No  data are available regarding the behavior of chloroform in  a
 POTW.  However, the biochemical oxidation of this compound was
 studied in one laboratory scale study at concentrations higher
 than those expected to be contained by most municipal waste-
 waters.  After 5, 10, and 20 days no degradation of  chloroform
                                183

-------
                                           I
 was observed.  The conclusion reached is that biological treat-
 ment produces little or no removal by degradation of chloroform
 in a POTW.

 The high vapor pressure of chloroform is expected to result in
 volatilization of the compound from aerobic treatment steps in a
 POTW.   Remaining chloroform is expected to pass through into the
 POTW effluent.

 Ethylbenzene (38).   Ethylbenzene is a colorless, flammable liquid
 manufactured commercially from benzene and ethylene.  Approxi-
 mately half of the  benzene used in the U.S. goes into the manu-
 facture of more^than three million tons of ethylbenzene annually.
 Ethylbenzene boils  at 136°C and has a vapor pressure of 7 mm Hg
 at 20  C.   It is slightly soluble in water (0.14 g/1 at 15°C) and
 is very soluble in  organic solvents.

 About  98 percent  of the ethylbenzene produced in the U.S.  goes
 into the production of styrene,  much of which is used in the
 plastics  and- synthetic rubber industries.  ! Ethylbenzene is a con-
 stituent of xylene  mixtures used as diluents in the paint  indus-
 try, agricultural insecticide sprays,  and gasoline blends.
                                           i
 Although humans are exposed to ethylbenzene from a variety of
 sources in the environment, little information on effects  of
 ethylbenzene in man or animals is  available.   Inhalation can
 irritate  eyes,  affect the  respiratory tract,  or cause vertigo.
 In laboratory animals ethylbenzene exhibited low toxicity.   There
 are no  data available on teratogenicity,  mutagenicity,  or  car-
 cinogenicity of ethylbenzene.

 Criteria  are based  on data derived from  inhalation exposure
 limits.   For the  protection of human health from the toxic  prop-
 erties  of ethylbenzene  ingested  through water  and  contaminated
 aquatic organisms,  the  ambient water quality  criterion  is  1.1
 mg/1.                                      ;

 The behavior of ethylbenzene  in  a  POTW has  not  been  studied in
 detail.   Laboratory  scale  studies  of the biochemical oxidation  of
 ethylbenzene  at concentrations greater than would  normally  be
 found in  municipal wastewaters have  demonstrated varying degrees
of degradation.   In one  study with phenol-acclimated seed
 cultures,  27 percent  degradation was observed  in a half day at
 250 mg/1  ethylbenzene.   Another  study at unspecified conditions
showed 32,  38, and 45 percent  degradation after  5, 10, and  20
days, respectively.   Based  on  these  results and  general observa-
tions relating molecular structure of degradation, the conclu-
sion is reached that biological treatment produces only mod-
erate removal of ethylbenzene  in a POTW by degradation.
                               184

-------
Other studies suggest that most of the ethybenzene entering  a
POTW is removed from the aqueous stream to the sludge.  The
ethylbenzene contained in the sludge removed  from the POTW may
volatilize.

Methylene Chloride (44).  Methylene chloride, also called dichlo-
romethane ' (CH?Cl2), is a colorless liquid manufactured by
chlorination of methane or methyl chloride followed by separation
from the higher chlorinated methanes formed as coproducts.
Methylene chloride boils at 40°C, and has a vapor pressure ofQ362
mm Hg at 20°C.  It is slightly soluble in water  (20 g/1 at 20 C) ,
and very soluble in organic solvents.  U.S. annual production is
about 250,000 tons.

Methylene  chloride is a common industrial solvent found in
insecticides, metal cleaners, paint, and paint and varnish
removers.

Methylene  chloride is not generally regarded  as  highly toxic to
humans.  Most human toxicity data are for exposure by inhalation.
Inhaled  methylene chloride acts as a central  nervous  system
depressant.  There is also evidence that the  compound causes
heart failure when large amounts are inhaled.

Methylene  chloride does produce mutation in tests for this
effect.  In addition, a bioassay recognized for  its extremely
high sensitivity to strong and weak carcinogens  produced  results
which were marginally significant.  Thus potential  carcinogenic
effects  of methylene chloride are not confirmed  or  denied,, but
are under  continuous study.  Difficulty in  conducting and inter-
preting  the test results from the low boiling point  (40 C)  of
methylene  chloride which increases the difficulty ofQmaintaining
the compound  in growth  media during incubation at 37  C; and  from
the difficulty of removing all impurities,  some  of which  might
themselves be carcinogenic.

For the  protection of human health  from the toxic properties of
methylene  chloride ingested through water  and contaminated
aquatic  organisms, the  ambient water criterion is 0.002 mg/1.
The behavior  of methylene chloride  in a POTW  has not  been studied
in any detail.  However, the biochemical  oxidation  of this com-
pound was  studied  in one laboratory scale  study at  concentrations
higher than  those  expected  to be  contained by most  municipal
wastewaters.  After  five days no  degradation  of methylene^chlo-
ride was observed.   The conclusion  reached is that .biological
treatment  produces little or no  removal by degradation  of
methylene  chloride in  a POTW.

The high vapor  pressure of  methylene  chloride is expected to
result in  volatilization of  the  compound  from aerobic treatment
steps  in a POTW.   It has been  reported  that methylene chloride
                                185

-------
 Inhibits  anerobic processes in a POTW.   Methylene chloride that
 is  not  volatilized in the POTW 'is expected to pass through into
 the effluent.

 Naphthalene  (55).   Naphthalene is an aromatic hydrocarbon with
 two orthocondensed benzene rings and a  molecular formula of
 ClO^S'  As such It is properly classed  as a polynuclear
 aromatic  hydrocarbon (PAH).   Pure naphthalene is a white crystal-
 line solid melting at 80°C.   For a solid, it has a relatively
 high vapor pressure (0.05 mm Hg  at 20°C), and moderate water
 solubility (19  mg/1 at 20°C).  Napthalene is the most abundant
 single  component  of coal  tar.  Production is more than a third of
 a million tons  annually in the U.S.   About three fourths of the
 production is used as feedstock  for  phthalic anhydride manufac-
 ture.   Most  of  the remaining production goes into manufacture of
 insecticide, dyestuffs, pigments,  and pharmaceuticals.  Chlori-
 nated and partially hydrogenated naphthalenes are used in some
 solvent mixtures.   Naphthalene is  also  used as a moth repellent.

 Naphthalene, ingested by  humans,  has reportedly caused vision
 loss  (cataracts),  hemolytic anemia,  and occasionally, renal dis-
 ease.   These effects  of naphthalene  ingestion are confirmed by
 studies on laboratory animals.  No carcinogenicity studies are
 available which can be used to demonstrate carcinogenic activity
 for naphthalene.   Naphthalene  does bioconcentrate in aquatic
 organisms.
                                            !
 For the protection of human health from the toxic properties of
 naphthalene  ingested through water and  through contaminated
 aquatic organisms,  the ambient water criterion is determined to
 be  143  mg/1.

 Only  a  limited  number of  studies have been conducted to determine
 the effects of  naphthalene on  aquatic organisms.   The data from
 those studies show only moderate  toxicity.

Naphthalene has been  detected  in  sewage plant effluents at con-
 centrations up  to  0.022 mg/1 in  studies carried out  by the U.S.
 EPA.  Influent  levels  were not reported.   The behavior of naph-
 thalene in a POTW  has  not  been studied.   However,  recent studies
have  determined that  naphthalene will accumulate  in  sediments at
 100 times the concentration  in overlying water.   These results
 suggest that naphthalene will  be readily removed  by  primary and
 secondary settling in  a POTW,  if it  is  not  biologically degraded.

Biochemical oxidation  of many  of the toxic  organic pollutants has
been  investigated  in  laboratory  scale studies  at  concentrations
higher  than would  normally be  expected  in municipal  wastewaters.
General observations  relating  molecular structure to ease of
degradation have been  developed  for  all of  these  pollutants.   The
                               186

-------
conclusion reached by study of the limited data is that biologi-
cal treatment produces a high removal by degradation of naphthal-
ene.  One recent study has shown that microorganisms can degrade
naphthalene, first to a dihydro compound, and ultimately to
carbon dioxide and water.

N-nitrosodiphenylamine (62).  N-nitrosodiphenylamine
UCfiHOoNNOj, also called nitrous diphenylamide, is a
yellow crystalline solid manufactured by nitrosation of diphenyl-
amine.  It melts at 66°C and is insoluble in water, but soluble
in  several organic solvents other than hydrocarbons.   Production
in  the U.S. has approached 1,500 tons per year.  The compound  is
used as a retarder for rubber vulcanization and as a pesticide
for control of scorch  (a fungus disease of plants).

N-nitroso compounds are acutely toxic to every animal  species_
tested and are also poisonous to humans.  N-nitrosodiphenylamine
toxicity in adult rats lies in the mid range of the values  for 60
N-nitroso compounds tested.  Liver damage is the principal  toxic
effect.  N-nitrosodiphenylamine, unlike many other N-nitroso-
amines, does not  show  mutagenic activity.  N-nitrosodiphenylamine
has been reported by several investigations to be non-carcino-
genic.  However,  the compound is capable of trans-nitrosation  and
could thereby convert  other amines to carcinogenic N-nitroso-
amines.  Sixty-seven of  87 N-nitrosoamines studied were  reported
to  have carcinogenic activity.  No water quality  criterion  have
been  proposed for N-nitrosodiphenylamine.

No  data are  available  on  the behavior of N-nitrosodiphenylamine
in  a  POTW.   Biochemical  oxidation  of many of  the  toxic organic
pollutants have been  investigated, at least  in  laboratory scale
studies, at  concentrations higher  than  those  expected  to be con-
tained  in  most municipal  wastewaters.    General  observations have
been  developed relating  molecular  structure  to  ease  of degrada-
tion  for  all the  toxic organic  pollutants.   The  conclusion
reached by  study  of  the  limited data is  that  biological  treatment
produces  little  or no  removal  of N-nitrosodiphenylamine in a
POTW.   No  information  is  available regarding possible  interfer-
ence  by N-nitrosodiphenylamine  in POTW  processes,  or on the
possible  detrimental  effect  on  sludge used  to amend soils in
which crops  are  grown.  However,  no  interference or detrimental
effects  are expected  because N-nitroso  compounds are widely dis-
tributed  in the  soil  and water  environment,  at low concentra-
tions,  as  a resu t  of microbial action  on nitrates  and
nitrosatable compounds.

Phthalate Esters (66-71).  Phthalic acid,  or 1,2-benzene-
 dicarboxylic acid,  is one of three isomeric benzenedicarboxylic
 acids produced by the chemical industry.   The other two isomeric
 forms are called isophthalic and terephthalic acids.  The formula
 for all three acids is C6H4(COOH)2-   Some esters of
                                187

-------
 phthalic acid are designated as toxic pollutants.  They will be
 discussed as a group here, and specific properties of individual
 phthalate esters will be discussed afterwards.

 Phthalic acid esters are manufactured in the U.S. at an annual
 rate in excess of one billion pounds.  They: are used as plasti-
 cizers - primarily in the production of polyvinyl chloride (PVC)
 resins.  The most widely used phthalate plasticizer is bis
 (2-ethylhexyl) phthalate (66) which accounts for nearly one-third
 of the phthalate esters produced.   This particular ester is com-
 monly referred to as dioctyl phthalate (DOP) and should not be
 confused with one of the less used esters, di-n-octyl phthalate
 (69), which is also used as a plasticizer.  In addition to these
 two isomeric dioctyl phthalates,  four other esters, also used
 primarily as plasticizers, are designated as toxic pollutants.
 They are:   butyl benzyl phthalate  (67), di-n-butyl phthalate
 (68), diethyl phthalate (70), and  dimethyl phthalate (71).

 Industrially, phthalate esters are prepared from phthalic anhy-
 dride and  the specific alcohol to  form the ester.   Some evidence
 is available suggesting that phthalic acid esters also may be
 synthesized by certain plant and animal tissues.   The extent to
 which this occurs in nature is not known.

 Phthalate  esters used as plasticizers can  be present in concen-
 trations up to 60 percent of the total weight of the PVC plastic.
 The plasticizer is not linked by primary chemical bonds to the
 PVC resin.   Rather,  it is locked into the  structure of intermesh-
 ing polymer molecules and held by  van der  Waals forces.   The
 result  is  that the plasticizer is  easily extracted.   Plasticizers
 are responsible for the odor associated with new plastic toys or
 flexible sheet that  has been contained in  a sealed package.

 Although the phthalate esters are  not soluble or  are only very
 slightly soluble in  water,  they do migrate into aqueous  solutions
 placed  in  contact  with the  plastic.   Thus,  industrial facilities
 with tank  linings, wire and cable  coverings;,  tubing,  and sheet
 flooring of PVC  are  expected to discharge  some  phthalate esters
 in  their raw waste.   In addition to  their  use as  plasticizers,
 phthalate  esters  are  used in lubricating oils and  pesticide  car-
 riers.  These also  can contribute  to  industrial discharge of
 phthalate  esters.

 From  the accumulated  data on acute toxicity;in  animals,  phtha-
 late  esters  may be considered as having  a  rather  low order of
 toxicity.  Human  toxicity data  are limited. '•  It is  thought that
 the toxic  effects  of  the  esters is most  likely  due  to  one  of  the
metabolic products, in  particular  the  monoester.   Oral acute  tox-
 icity in animals  is greater  for the  lower  molecular  weight esters
than  for the higher molecular weight  esters.
                               188

-------
Orally administered phthalate esters.generally produced enlarging
of liver and kidney, and atrophy of testes in laboratory animals.
Specific esters produced enlargement of heart and brain, spleen-
itis, and degeneration of central nervous system tissue.

Subacute doses administered orally to laboratory animals produced
some decrease in growth and degeneration of the testes.  Chronic
studies in animals showed similar effects to those found in acute
and subacute studies, but to a much lower degree.  The same
organs were enlarged, but pathological changes were not usually
detected.

A recent study of several phthalic esters produced suggestive but
not conclusive evidence that dimethyl and diethyl phthalates have
a cancer liability.  Only four of the six toxic pollutant  esters
were included in the study.  Phthalate esters do bioconcentrate
in fish.  The factors, weighted  for relative consumption of
various aquatic and marine food  groups, are used to calculate
ambient water quality criteria for four phthalate esters.  The
values are included in the discussion of the specific  esters.

Studies of toxicity of phthalate esters in freshwater  and  salt
water organisms are scarce.  A chronic toxicity test with  bis (2-
ethylhexyl) phthalate showed that significant reproductive
impairment occurred at 0.003 mg/1 in the freshwater crustacean,
Daphnia magna.  In acute toxicity studies, saltwater  fish  and
organisms showed sensitivity differences of up to eight-fold  to
butyl benzyl, diethyl, and dimethyl phthalates.  This  suggests
that each ester must be evaluated individually for toxic effects.

The behavior  of phthalate esters in  a POTW has not been  studied.
However, the biochemical oxidation of many of the toxic  organic
pollutants has been  investigated in  laboratory scale  studies_at
concentrations higher than would normally, be expected  in munici-
pal wastewaters.  Three of the phthalate esters were  studed.
Bis(2-ethylhexyl) phthalate was  found to be degraded  slightly or
not  at  all  and its  removal by biological treatment  in a POTW is
expected to be slight or zero.   Di-n-butyl phthalate  and diethyl
phthalate were degraded to a moderate degree  and  their removal by
biological  treatment  in a POTW is expected to  occur  to a moderate
degree.  Using these  data and other  observations  relating  molecu-
lar  structure  to ease of biochemical degradation  of  other  toxic
organic  pollutants,  the conclusion was  reached  that  butyl  benzyl
phthalate and dimethyl phthalate would  be  removed  in  a POTW to a
moderate degree by  biological  treatment.   On  the  same basis,  it
was  concluded that  di-n-octyl phthalate  would  be  removed to a
slight  degree or  not at all.  An EPA study of seven  POTW facili-
ties  revealed that  for  all but di-n-octyl  phthalate,  which was
not  studied,  removals  ranged  from 62 to 87 percent.
                                189

-------
No  information was  found on possible interference with POTW oper-
ation  or  the  possible  effects  on sludge by the phthalate esters.
The water insoluble phthalate  esters - butyl benzyl and di-n-
octyl  phthalate - would  tend to  remain in sludge, whereas the
other  four toxic pollutant  phthalate esters with water solubili-
ties ranging  from 50 mg/1 to 4.5 mg/1 would probably pass through
into the  POTW effluent.
                                          i
Bis(2-ethylhexyl) phthalate (66).   In addition to the general
remarks and discussion on phthalate esters, specific information
on  bis(2-ethylhexyl) phthalate is  provided.  Little information
is  available  about  the physical  properties of bis(2-ethylhexyl)
phthalate.  It is a liquid  boiling at 387°C at 5mm Hg and is
insoluble in  water.  Its  formula is CgH^COOCgHiy^-
This toxic pollutant constitutes about one-third of the phthalate
ester  production in the  U.S.   It is commonly referred to as
dioctyl phthalate,  or  DOP,  in  the  plastics industry where it is
the most  extensively used compound for the plasticization of
polyvinyl chloride  (PVC).   Bis(2-ethylhexyl) phthalate has been
approved  by the FDA for  use in plastics in contact with food.
Therefore,  it may be found  in  wastewaters coming in contact with
discarded plastic food wrappers  as well as the PVC films and
shapes normally found  in industrial plants.  This toxic pollutant
is  also a commonly  used  organic  diffusion pump oil,  where its  low
vapor  pressure is an advantage.

For the protection  of  human health from the toxic properties of
bis(2-ethylhexyl) phthalate ingested through water and through
contaminated  aquatic organisms,  the ambient water quality criter-
ion is determined to be  15  mg/1.   If contaminated aquatic organ-
isms alone  are consumed,  excluding the consumption of water, the
ambient water criteria is determined to be 50 mg/1.

Although  the  behavior  of  bis(2-ethylhexyl)  phthalate  in a POTW
has not been  studied,  biochemical  oxidation of this  toxic pollu-
tant has  been studied  on  a  laboratory scale at concentrations  "
higher than would normally  be  expected in municipal  wastewater.
In  fresh  water  with a  non-acclimated seed culture no  biochemical
oxidation was  observed after 5,  10,  and 20 days.   However,  with
an  acclimated seed culture, biological oxidation occured to the
extents of  13,  0, 6, and  23 percent of theoretical after 5,  10,
15  and 20 days,  respectively.  Bis(2-ethylhexyl)  phthalate
concentrations  were 3  to  10 mg/1.   Little or no  removal of
bis(2-ethylhexyl) phthalate by biological treatment  in a POTW  is
expected.

Butyl benzyl  phthalate (67).   In addition to the  general remarks
and discussion  on phthalate esters,  specific information on butyl
benzyl phthalate is provided.  No  information was found on the
physical  properties of this compound.
                               190

-------
Butyl benzyl phthalate is used as a plasticizer for PVC.  Two
special applications differentiate it from other phthalate
esters.  It is approved by the U.S. FDA for food contact in
wrappers and containers; and it is the industry standard_for
plasticization of vinyl flooring because it provides stain
resistance.

No ambient water quality criterion is proposed for butyl benzyl
phthalate.

Butyl benzyl phthalate removal in a POTW by biological  treatment
is expected to occur to a moderate degree.

Pi-n-butyl phthalate  (68).   In addition to the general  remarks
and discussion on phtESTate  esters, specific  information on  di-
n-butyl phthalate (DBF) is provided,  DBF is  a colorless, oil
liquid, boiling at  3406C.  Its water  solubility at room tempera-
ture is reported to be 0.4 g/1 and 4.5 g/1 in two different  chem-
istry handbooks.  The formula  for DBF, CeH^COOCAHg^
is the  same as for  its isomer, di-isobutyl phthalate.   DBF
production  is 1 to  2 percent of  total U.S. phthalate ester
production.

Dibutyl phthalate is used to a limited extent as  a plasticizer
for polyvinyl chloride  (PVC).  It  is  not  approved for  contact
with food.  It is used in liquid lipsticks and  as  a  diluent  for
polysulfide dental  impression  materials.   DBF is  used  as a  plas-
ticizer for nitrocellulose  in  making  gun  powder,  and as a  fuel in
solid  propellants  for rockets.   Further uses  are  insecticides,
safety glass manufacture, textile  lubricating agents,  printing
inks,  adhesives, paper coatings, and  resin solvents.

For  protection  of human  health from the  toxic properties of
dibutyl phthalate  ingested  through water  and  through contami-
nated  aquatic  organisms,  the ambient  water quality criterion is
determined to be  34 mg/1.   If  contaminated aquatic organisms
alone  are consumed, excluding  the consumption of water, the
ambient water  criterion  is  154 mg/1.

Although the  behavior of di-n-butyl phthalate in a POTW has not
been studied,  biochemical oxidation of this toxic pollutant has
been studied  on a laboratory scale at concentrations higher than
would  normally be expected in municipal wastewaters.  Biochemical
 oxidation of 35,  43, and 45 percent of theoretical oxidation were
 obtained after 5,  10, and 20 days, respectively,  using sewage
 microorganisms  as an unacclimated seed culture.

 Biological treatment in a POTW is expected to. remove di-n-butyl
 phthalate to a moderate degree.
                                191

-------
                                            ••}!•	r'f!11"1-'":1"'" :'. Itli''?•'' '"I11!	''
                                                                 ., BPf . if,"I	i
 Di-n-octyl phthalate  (69) .  In addition  to  the  general  remarks
 and discussion on phthalate esters, specific  information  on
 di-n-octyl phthalate  is provided.  Di-n-octyl phthalate is not  to
 be confused with the  isomeric bis (2-ethylhexyl) phthalate which
 is commonly referred  to in the plastics  industry as  DOP.  Di-n-
 octyl phthalate is a  liquid which boils  at  220°C at  5 mm  Hg.  It
 is insoluble in water.  Its molecular  formula is CgH/^-
 (COOCgHiy^-  Its production constitutes about  1 percent  of
 all phthalate ester production in the  U.S;

 Industrially, di-n-octyl phthalate is  used  to plasticize  poly-
 vinyl chloride (PVC) resins.

 No ambient water quality criterion is  proposed  for di-n-octyl
 phthalate .

 Biological treatment in a POTW is expected  to lead to little or
 no removal of di-n-octyl phthalate.
                       J  *               \ [[[

 Dimethyl phthalate (71).  In addition  to the general remarks and
 discussion on phthalate esters, specific information on dimethyl
 phthalate (BMP)  is provided.   BMP has  the lowest molecular weight
 of the phthalate esters - M.W.  = 194 compared to M.W. of  391 for
 bis (2-ethylhexyl)  phthalate.   DMP has a boiling point of  282°C.
 It is a colorless  liquid,  soluble in water  to the extent  of 5
 mg/1.   Its molecular formula is
 Dimethyl  phthalate production in the U.S. iis just under one per-
 cent  of total phthalate ester production.  DMP is used to some
 extent  as a  plasticizer in cellulosics ; however, its principal
 specific  use is  for dispersion of polyvinylidene fluoride (PVDF) .
 PVDF  is resistant  to most chemicals and finds use as electrical
 insulation,  chemical process  equipment (particularly pipe) , and
 as a  case for long-life finishes for exterior metal siding.  Coil
 coating techniques are  used to apply PVDF dispersions to aluminum
 or galvanized steel siding.

 For the protection of human health from the toxic properties of
 dimethyl  phthalate ingested through water iand through contami-
 nated aquatic organisms,  the  ambient water criterion is deter-
 mined to  be  313 mg/1.   If contaminated aquatic organisms alone
 are consumed,  excluding the consumption of water, the ambient
 water criterion is  2,900 mg/1.

 Based on  limited data and observations relating molecular struc-
 ture to ease  of biochemical degradation of other toxic organic
 pollutants,  it is  expected that  dimethyl phthalate will be bio-

-------
Polynuclear Aromatic Hydrocarbons  (72-84).  The polynuclear aro-
matic hydrocarbons(PAH) selected as toxic pollutants are a group
of 13 compounds consisting of substituted and unsubstituted poly-
cyclic aromatic rings.  The general class of PAH includes hetero-
cyclics, but none of those were selected  as toxic pollutants.
PAH are formed as the result of incomplete combustion when
organic compounds are burned with insufficient oxygen.   PAH are
found in coke oven emissions, vehicular emissions, and volatile
products of oil and gas burning.  The compounds chosen as toxic
pollutants are listed with their structural formula and  melting
point (m.p.).  All are insoluble in water.
     72

     73

     74

     75


     76

     77


     78

     79


     80

     81

     82


     83
Benzo(a)anthracene (1,2-benzanthracene)

Benzo(a)pyrene (3,4-benzopyrene)

3,4-Benzofluoranthene
   m.p,

   m.p,

   m. p,
162°C

176°C

168°C
Benzo(k)fluoranthene (11,12-benzofluoranthene)
                                             m.p
Chrysene (1,2-benzphenanthrene)

Acenaphthylene
     HC=GH

Anthr.acene

Benzo(ghi)perylene (1,12-benzoperylene)
                                      m.p <

Fluorene (alpha-diphenylenemethane)

Phenanthrene

Dibenzo(a,h)anthracene  (1,2,5,6-
             dibenzoanthracene)
Indeno (1,2,3-cd)pyrene
 (2,3-o-phenylenepyrene)
                                                m.p.
         217°C

   m.p.255°C

   m.p,
92 °C
     84   Pyrene
    m.p.  216°C


,  not  reported

    m.p.  116°C

    m.p.  101°C


    m.p.  269°C


not available

    m.p.  156°C
                                193

-------
 Some  of these  toxic  pollutants  have commercial or industrial
 uses.   Benzo(a)anthracene,  benzo(a)pyrene,  chrysene,  anthracene,
 dibenzo(a,h)anthracene,  and pyrene are all  used as antioxidants.
 Chrysene, acenaphthylene,  anthracene,  fluorene, phenanthrene,  and
 pyrene  are  all used  for  synthesis  of dyestuffs or other organic
 chemicals.  3,4-Benzofluoranthrene,  benzo(k)fluoranthene,  benzo-
 (ghi)perylene, and indeno  (1,2,3-cd)pyrene  have no known indus-
 trial uses, according  to the results of a recent literature
 search.                                    \

 Several of  the PAH toxic pollutants  are found in smoked meats,  in
 smoke flavoring mixtures,  in vegetable oils,  and in coffee.  Con-
 sequently,  they are  also found  in  many drinking water supplies.
 The wide distribution  of these  pollutants in  complex  mixtures
 with  the many  other  PAHs which  have  not been  designated as toxic
 pollutants  results in  exposures  by humans that cannot be associ-
 ated with specific individual compounds.

 The screening  and verification  analysis procedures used for the
 toxic organic  pollutants are based on  gas chromatography (GC).
 Three pairs of the PAH have identical  elution times on the column
 specified in the protocol,  which meansvthat the parameters of  the
 pair are not differentiated.  For  these three pairs [anthracene
 (78)  -  phenanthrene (81);  3,4-benzofluoranthene (74)  - benzo(k)-
 fluoranthene (75); and benzo(a)anthracene (72) - chrysene  (76)]
 results  are obtained and reported  as "either-or."  Either  both
 are present in the combined concentration reported, or one is
 present  in  the concentration reported.

 There are no studies to  document the possible carcinogenic risks
 to humans by direct  ingestion.   Air  pollution studies  indicate  an
 excess of lung cancer  mortality  among  workers exposed  to large
 amounts  of  PAH containing materials  such  as coal gas,  tars,  and
 coke-oven emissions.   However, no  definite proof exists  that the
 PAH present in these materials  are responsible for the cancers
 observed.
                                           1
Animal studies have demonstrated the toxicity of PAH by  oral and
 dermal administration.   The  carcinogenicity of PAH has been
 traced to formation of PAH  metabolites  which,  in turn,  lead  to
 tumor formation.   Because the levels of PAHj which induce cancer
 are very low,   little work has been done on other  health  hazards
resulting from exposure.  It has been  established in  animal
 studies that tissue damage  and systemic toxicity  can result  from
exposure to non-carcinogenic PAH compounds.
                               194

-------
Because there were no studies available regarding chronic oral
exposures to PAH mixtures, proposed water quality criteria were
derived using data on exposure to a single compound.  Two studies
were selected, one involving benzo(a)pyrene ingestion and one
involving dibenzo(a,h)anthracene ingestion.  Both are known
an imal c ar c ino gen s.

For the maximum protection of human health from the potential
carcinogenic effects of expsure to polynuclear aromatic hydrocar-
bons (PAH) through ingestion of water and contaminated aquatic
organisms, the ambient water concentration is zero.  Concentra-
tions of PAH estimated to result in additional risk of 1  in
100,000 were derived by the EPA and the Agency is^considering
setting criteria at an interim target risk level  in the range of
10~7  10~°, or 10~5 with corresponding criteria of
0.000000097 mg/1, 0.00000097 mg/1, and 0.0000097  mg/1,
respectively.

No  standard toxicity tests have been reported  for freshwater or
saltwater organisms and any of the 13 PAH discussed here.

The behavior of PAH in a  POTW has received only a limited amount
of  study.   If  is reported  that up to 90 percent of  PAH entering  a
POTW will be retained in  the sludge generated by  conventional
sewage  treatment processes.  Some of the  PAH can  inhibit  bac-
terial  growth  when they are present at concentrations  as^low as
0.018 mg/1.   Biological treatment in activated  sludge  units  has
been shown  to  reduce the  concentration of phenanthrene^and
anthracene  to  some  extent; however,  a  study  of biochemical oxi-
dation  of  fluorene on a laboratory  scale  showed no  degradation
after  5,  10,  and  20 days.   On  the basis  of that  study  and studies
of  other  toxic organic pollutants,  some  general  observations were
made relating molecular  structure  to  ease of degradation.  Those
observations  lead  to  the  conclusion  that  the 13 PAH selected to
represent that group  as  toxic  pollutants  will  be  removed °nly
slightly or not at all by biological  treatment methods in a POTW.
Based  on their water  insolubility and  tendency to attach to sedi-
ment particles very little pass  through of PAH to POTW effluent
 is  expected.

No  data are available at  this  time to support any conclusions
 about  contamination of land by PAH on which sewage sludge con-
 taining PAH is spread.

 Tetrachloroethylene (85).  Tetrachlorbethylene (CC12CC12),
 also called perchloroethylene and PCE, is a colorless, nonflam-
 mable liquid, produced mainly by two methods - chlorination  and
 pyrolysis of ethane and propane, and oxychlorination of dichloro-
 ethane.  U.S. annual production exceeds 300,000 tons.  PCE  boils
 at 121°C and has a vapor pressure of 19 mm Hg at 20 C.   It  is
 insoluble in water but soluble in organic solvents.
                                195

-------
 Approximately two-thirds of the U;S. production  of PCE is used
 for dry cleaning.  Textile processing and! metal  degreasing,  in
 equal amounts consume about one-quarter of the U.S. production.

 The principal toxic effect of PCE on humans is central nervous
 system depression when the compound is inhaled.  Headache,
 fatigue, sleepiness, dizziness, and sensations of intoxication
 are reported.  Severity of effects increases with vapor concen-
 tration.  High integrated exposure (concentration times duration)
 produces kidney and liver damage.  Very limited  data on PCE
 ingested by laboratory animals indicate liver damage occurs when
 PCE is administered by that route.  PCE tends to distribute to
 fat in mammalian bodies.

 One report found in the literature suggests, but does not con-
 clude, that PCE is teratogenic.   PCE has been demonstrated to be
 a liver carcinogen in B6C3-F1 mice.

 For the maximum protection of human health from the potential
 carcinogenic effects  of exposure to tetrachlorethylene through
 ingestion of water and contaminated aquatic organisms, the ambi-
 ent water concentration is  zero.   Concentrations of tetrachloro-
 ethylene estimated to result in  additional lifetime cancer risk
 levels of 10- ',  ICT5,  and 10~5 are 0.000020 mg/1, 0.00020
 mg/1,  and 0.0020 mg/1,  respectively.

 No  data were found regarding the  behavior  of PCE in a POTW.   Many
 of  the toxic organic  pollutants have  been  investigated,  at least
 in  laboratory scale studies,  at  concentrations  higher than those
 expected  to  be  contained by  most  municipal wastewaters.   General
 observations have been  developed  relating  molecular structure to
 ease of  degradation for  all  of the toxic organic  pollutants.   The
 conclusions  reached by  the study  of the  limited data  is  that
 biological treatment produces  a moderate removal  of PCE  in a  POTW
 by  degradation.   No information was found  to  indicate  that PCE
 accumulates  in the  sludge, but some PCE is expected to be   -
 adsorbed  onto settling particles.   Some PCE is  expected  to be
 volatilized  in aerobic treatment processes! and  little, if  any,  is
 expected  to  pass  through into  the  effluent from the POTW.
Toluene
  Toluene is a clear, colorless liquid with a
odor.  It is a naturally occuring compound derived
                                         Some
benzene
primarily from petroleum or petrochemical processes. __
toluene is obtained from the manufacture of "metallurgical  coke.
Toluene is also referred to as totuol, methylbenzene ,  methacide.
and phenylme thane.  It is an aromatic hydrocarbon with the
formula C6H5CH3.  It boils at 111°C and has a vapor pres-
sure of 30 mm Hg at room temperature.  The water solubility of
toluene is 535 mg/1, and it is miscible with a variety of organic'
solvents.  Annual production of toluene in the U.S. is greater
than two million metric tons.  Approximately two-thirds of the
                               196

-------
toluene is converted to benzene 'and the remaining 30 percent is
d?v?ded approximately equally into chemical manufacture, and  use
as a paint solvent and aviation gasoline additive.  An esti-
mated 5,000 metric tons is discharged to the environment anually
as a constituent in wastewater.

Most data on the effects of toluene in human and other mammals
have been based on inhalation exposure or dermal contact studies.
There appear to be no reports of oral administration of toluene
SnumS Subjects.  A long term toxicity study  on female rats
revealed no adverse effects on growth, mortality, appearance  and
behavior, organ to body weight ratios, blood-urea nitrogen
leveTsTboneSmarrow counts, peripheral blood counts, or morphol-
ogy of major organs.  The effects  of  inhaled toluene_on the cen-
tral nervous system, both at high  and low concentrations,  have  ^
blen studied in humans and animals.   However   ingested  toluene  is
expected to be handled differently by the body because  it  is
absorbed more slowly and must  first pass through  the  liver before
reaching the nervous system.   Toluene is extensively  and  rapidly
metabolized in the  liver.  One of  the principal metabolic  prod-
ucts of toluene  is  benzoic acid, which  itself  seems  to  have
little potential  to produce  tissue injury.

Toluene does not  appear  to be  teratogenic  in laboratory animals
or man.  Nor  is  there  any  conclusive  evidence  that  toluene is
mutagenic.  Toluene has  not  been demonstrated  to  be positive in
any in vitro  mutagenicity  or carcinogenicity bioassay system, nor
to be  carcinogenic  in  animals  or man.

Toluene has been found in  fish caught in harbor waters in the
vicinity  of petroleum and  petrochemical plants.  Bioconcentration
Itudies have  not been conducted, but  bioconcentration factors
have been calculated on the  basis of the octanol-water partition
 coefficient.

 For the  protection of human health from the toxic properties of
 toluene ingested through water and through contaminated aquatic
 organisms, the ambient water criterion is determined to be 14.3
 me/1   If contaminated aquatic organisms alone are consumed
 excluding £he consumption of water, the ambient water criterion
 is 424 mg/1.   Available data show that the adverse effects on
 aquatic life occur at concentrations as low as 5 mg/1.

 Acute toxicity tests have been conducted with  toluene and a
 variety of freshwater fish and Daphnia magna.  ^%la"^ *
 to be significantly more resistant tKIn-TTiK.  No test results
 have been reported for the chronic effects of  toluene on
 freshwater fish or invertebrate species.

 No detailed study of toluene behavior in a  POTW  is available.
 However,  the biochemical oxidation of many  of the  toxic  pollu-
 tants has been  investigated in  laboratory scale  studies  at
                                 197

-------
 concentrations greater  than  those  expected  to  be  contained  by
 most municipal wastewaters.  At  toluene  concentrations  ranging
 from 3 to 250 mg/1 biochemical oxidation proceeded  to 50  percent
 of theoretical or greater.   The  time period varied  from a few
 hours to 20 days depending on whether  or not the  seed culture was
 acclimated.  Phenol adapted  acclimated seed cultures gave the
 most rapid and extensive biochemical oxidation.

 Based on study of the limited data, it is expected  that toluene
 will be biochemically oxidized to a lesser  extent than  domestic
 sewage by biological treatment in a POTW.   The volatility and
 relatively low water solubility of toluene  lead to  the  expecta-
 tion that aeration processes will remove  significant quantities
 of toluene from the POTW.  The EPA studied  toluene  removal  in
 seven POTW facilities.  The removals ranged from 40 to  100
 percent.   Sludge concentrations of toluene ranged from  54 x
 10~J to 1.85 mg/1.

 Trichloroethylene (87^.   Trichloroethylene  (1,1,2-trichloroethyl-
 ene  or TCE)  is  a clear,  colorless liquid boiling at 87°C.   It has
 a  vapor pressure of 77 mm Hg at room temperature and is slightly
 soluble in water (1 gm/1).   U.S.  production is  greater than 0.25
 million metric  tons annually.  It is produced from  tetrachloro-
 ethane  by treatment with lime in  the presence of water.

 TCE  is  used  for  vapor  phase  degreasing  of metal parts,  cleaning
 and  drying electronic  components, as a  solvent  for paints, as a
 refrigerant,  for  extraction  of  oils,  fats, and  waxes,  and  for dry
 cleaning.  Its widespread use and relatively high volatility
 result  in detectable levels  in  many parts of the environment.

 Data on the effects produced  by ingested  TCE are limited.  Most
 studies have been directed at inhalation  exposure.   Nervous  sys-
 tem disorders and liver  damage  are  frequent  results  of  inhalation
 exposure.  In the short  term  exposures, TCE  acts  as  a  central
 nervous system depressant - it was  used as an anesthetic before
 its other long term effects were  defined.

 TCE has been shown to  induce  transformation  in  a highly  sensitive
 J§ vltro Fischer  rat embryo cell  system (F1706)  that is  used for
 identifying carcinogens.  Severe  and persistent  toxicity to  the
 liver was recently demonstrated when TCE  was shown to produce
 carcinoma of the  liver in mouse strain B6C3F1.  One  systematic
 8tud.y of TCE exposure and the incidence of human cancer  was  based
on 518 men exposed to TCE.  The authors of that  study concluded
that although the cancer risk to man cannot  be ruled out,  expo-
sure to low levels of TCE probably does not  present  a very
serious and general cancer hazard.
                               198

-------
TCE is bioconcentrated in aquatic species, making the consumption
of such species by humans a significant source of TCE.  For the
protection of human health from the potential carcinogenic
effects of exposure to trichloroethylene through ingestion of
water and contaminated aquatic organisms, the ambient water con-
centration is zero.  Concentrations of trichloroethylene e^tx-
mated to result in additional lifetime cancer risks of 10   ,
10-6, and 10-5 are 2.7 x lO'4 mg/1, 2.7 x 10 •* mg/1, and
2 7 x 10'2 mg/1, respectively.  If contaminated aquatic organ-
isms alone are consumed, excluding the consumption of water  the
water concentration should be less than 0.807 mg/1 to keep  the
additional lifetime cancer risk below 10~3.

Only a very  limited amount of data on the effects of TCE on
freshwater aquatic life  are  available.  One  species of  fish (fat-
head minnows)  showed a loss  of equilibrium at concentrations
below those  resulting in lethal effects.

The behavior of trichloroethylene in  a POTW  has  not been  studied.
However,  in  laboratory scale studies  of  toxic organic PollutantB,
TCE was  subjected  to biochemical  oxidation  conditions.  Alter  i,
10  and  20 days no biochemical  oxidation  occurred.   On  the basis
of'this  study and  general  observations  relating molecular  struc-
ture  to  ease of degradation, the  conclusion  is  reached  that TCE
would undergo no  removal by biological  treatment in a POTW.  The
volatility Snd relatively  low water  solubility  of TCE is  expected
to  result in volatilization of some  of the  TCE in aeration steps
in  a  POTW.

Antimony (114).   Antimony (chemical  name - stibium, symbol Sb) ,
classifiecns--a non-metal  or metalloid,  is.a silvery white, brit-
tle crystalline solid.   Antimony is  found in small ore bodies_
throughout the world.   Principal ores are oxides of mixed anti-
mony valences, and an oxysulfide ore.  Complex ores with metals
 are important because the antimony is recovered as a by-product.
 Antimony melts at 631°C, and is a poor conductor of electricity
 and heat.

 Annual U.S.  consumption of primary antimony ranges from 1,0,000 to
 20,000 tons.  About half is consumed in metal products - mostly
 antimonial  lead for lead acid storage batteries, *ndm^out half
 in non-metal products.  A principal compound is antimony trioxide
 which is used as a flame retardant in fabrics, and as an opaci-
 fier in glass, ceramics, and enamels.  Several antimony compounds
 are used as  catalysts in organic chemicals  synthesis, as  fluori-
 nating agents  (the antimony  fluoride), as pigments, and ^fire-
 works!  Semiconductor applications are economically significant.

 Essentially no information  on antimony-induced^human health
 effects has been derived  from community  epidemiology studies.
 The  available data are  in  literature relating  effects  observed
                                 199

-------
 with therapeutic or medicinal uses of antimony compounds and
 industrial  exposure studies.   Large therapeutic doses of anti-
 monial compounds, usually used to treat schistisomiasis, have
 caused severe nausea,  vomiting,  convulsions,  irregular heart
 action,  liver damage,  and skin rashes.  Studies of acute
 industrial  antimony poisoning have revealed loss of appetite,
 diarrhea, headache, and dizziness in addition to the symptoms
 found in studies of therapeutic  doses of antimony.
                                            i
 For  the  protection of  human health from the toxic properties of
 antimony ingested through water  and through contaminated aquatic
 organisms the ambient  water criterion is determined to be 0.146
 mg/1.   If contaminated aquatic organisms are  consumed, excluding
 the  consumption  of water,  the ambient water criterion is deter-
 mined to be 45 mg/1.   Available  data show that adverse effects on
 aquatic  life occur at  concentrations higher than those cited for
 human health risks.

 Very little information is available regarding the behavior of
 antimony in a POTW. The limited solubility of most antimony
 compounds expected in  a POTW, i.e.,  the oxides and sulfides, sug-
 gests  that  at least part of the  anfeimony entering a POTW will be
 precipitated and incorporated into the sludge.  However,  some
 antimony is  expected to remain dissolved and  pass through the
 POTW into the effluent.  Antimony compounds remaining in the
 sludge under anaerobic conditions may be connected to stibine
 (SbH3),  a very soluble and very  toxic compound.   There are no
 data to  show antimony  inhibits any POTW processes.   Antimony is
 not  known to be  essential  to  the growth of plants,  and has been
 reported to  be moderately  toxic.   Therefore,  sludge containing
 large  amounts of antimony could  be detrimental to plants  if it is
 applied  in  large  amounts to cropland.
                                            i	
Arsenic  (115).  Arsenic (chemical symbol As),  is  classified as a
non-metal or metalloid.   Elemental arsenic normally exists in the
alpha-crystalline  metallic form  which is steel gray and brittle,
and  in the beta  form which is dark gray and amorphous.   Arsenic
sublimes at  615°C.  Arsenic is widely distributed throughout the
world  in a  large  number of minerals.   The most important  commer-
cial source  of arsenic is  as  a by-product from treatment  of
copper,  lead,  cobalt,  and  gold ores.   Arsenic  is  usually  marketed
as the trioxide  (As2°3)-   Annual  U.S.  production  of the tri-
oxide approaches  40,000 tons.

The  principal  use  of arsenic  is  in agricultural  chemicals (herbi-
cides) for controlling weeds  in  cotton fields.  Arsenicals  have
various  applications in medicinal and  vetrinary use,  as wood
preservatives, and  in  semiconductors.
                                            i
The effects of arsenic  in  humans  were  known by the  ancient  Greeks
and Romans.   The principal  toxic  effects are gastrointestinal
                               200

-------
disturbances.  Breakdown of red blood cells occurs.  Symptoms of
acute poisoning include vomiting, diarrhea, abdominal pain,
lassitude, dizziness, and headache.  Longer exposure produced
dry, falling hair, brittle, loose nails, eczema, and exfoliation.
Arsenicals also exhibit teratogenic and mutagenic effects  in
humans.  Oral administration of arsenic compounds has been
associated clinically with skin cancer for nearly one hundred
years.  Since 1888 numerous studies have linked occupational
exposure and therapeutic administration of arsenic compounds to
increased incidence of respiratory and skin cancer.

For the maximum protection of human health from the potential
carcinogenic effects of exposure to arsenic through ingestion of
water and contaminated aquatic organisms, the ambient water con-
centration is zero.  Concentrations of arsenic estimated  to
result in additional lifetime cancer risk levels of 10~',
ID"6, and 1C)-5 are 2.2 x 1CT7 mg/1, 2.2 x 10"b mg/1, and
2.2 x 10"5 mS/1» respectively.  If contaminated aquatic organ-
isms alone are consumed, excluding the consumption of water, the
water concentration should be less than 1.75 x 10~^ to keep the
increased lifetime cancer risk below 10~5.  Available data show
that adverse effects on aquatic life occur at concentrations
higher than  those cited for human health risks.

A  few studies have been made regarding the behavior of  arsenic  in
a  POTW.  One EPA survey of nine POTW facilities reported  influent
concentrations ranging from 0.0005 to 0.693 mg/1; effluents  from
three a POTW having biological treatment contained  0.0004 to  0.01
mg/1; two POTW facilities  showed arsenic removal  efficiencies  of
50 and 71 percent in biological treatment.   Inhibition  of treat-
ment processes by sodium arsenate  is reported  to  occur  at 0.1
mg/1 in activated sludge,  and  1.6 mg/1 in  anaerobic digestion
processes.   In another study based'on data  from  60  POTW facili-
ties, arsenic in  sludge ranged  from  1.6 to  65.6  mg/kg  and the
median value was  7.8 mg/kg. Arsenic  in  sludge  spread  on cropland
may be taken up by plants  grown on that land.  Edible  plants  can
take up arsenic, but normally  their  growth is  inhibited before
the plants are ready for harvest.

Cadmium  (118).  Cadmium is a relatively rare  metallic  element
that  is selclom  found in  sufficient  quantities  in a pure state to
warrant mining  or extraction  from  the earth's  surface.   It^is
found  in  trace  amounts of  about  1  ppm  throughout the  earth s
crust.  Cadmium is, however, a valuable by-product  of zinc pro-
duction.

Cadmium  is used primarily  as  an electroplated metal,  and  is found
as an  impurity  in the  secondary refining  of zinc,  lead, and
copper.
                                201

-------
Cadmium  Is'an  extremely  dangerous  cumulative toxicant,  causing
progressive  chronic  poisoning  in mammals,  fish,  and probably
other  organisms.   The  metal  is not excreted.

Toxic  effects  of  cadmium on  man have  been  reported from through-
out the  world.  Cadmium  may  be a factor  in the  development  of
such human pathological  conditions as kidney disease,  testicular
tumors,  hypertension,  arteriosclerosis,  growth  inhibition,
chronic  disease of old age,  and cancer.  Cadmium is normally
ingested by  humans through food and water  as  well as by breathing
air contaminated  by  cadmium  dust.   Cadmium is cumulative in the
liver,, kidney, pancreas,  and thyroid  of  humans  and other animals.
A severe bone  and kidney syndrome  known  as itai-itai disease has
been documented in Japan as  caused by cadmium ingestion via
drinking water and contaminated irrigation water.   Ingestion of
as little as 0.6  mg/day  has  produced  the disease.   Cadmium  acts
synergistically with other metals.  Copper and  zinc substantially
increase its toxicity.

Cadmium  is concentrated  by marine  organisms,  particularly
molluscs, which accumulate cadmium in calcareous tissues and in
the viscera.   A concentration  factor  of  1,000 for cadmium in fish
muscle has been reported, as have  concentration  factors of  3,000
in marine plants  and up  to 29,600  in  certain  marine animals.   The
eggs and larvae of fish  are  apparently more sensitive  than  adult
fish to  poisoning by cadmium,  and  crustaceans appear to be  more
sensitive than fish  eggs  and larvae.      j.

For the  protection of  human  health from  the toxic properties of
cadmium  ingested  through  water and  through contaminated aquatic
organisms, the ambient water criterion is  determined to be  0.010
mg/1.  Available  data  show that  adverse  effects  on aquatic  life
occur at concentrations  in the same range  as  those cited for
human health,  and  they are highly  dependent on water hardness.

Cadmium  is not destroyed  when  it is introduced into a  POTW,  and
will either  pass  through  to  the  POTW  effluent or be incorporated
into the POTW  sludge.  In addition, it can  interfere with the
POTW treatment process.

In a study of  189 POTW facilities,  75 percent of the primary
plants,  57 percent of  the trickling filter!  plants,  66 percent of
the activated  sludge plants, and 62 percent of the biological
plants allowed over  90 percent of  the influent cadmium  to pass
through  to the POTW  effluent.   Only two  of  the 189 POTW facili-
ties allowed less than 20 percent pass-through,  and none less
than 10  percent pass-through.   POTW effluent  concentrations
ranged from  0.001 to 1.97 mg/1  (mean  0.028  mg/1,  standard
deviation 0.167 mg/1).
                               202

-------
   -rpA«ses  the  level of cadmxuia i_n tne so3.i*   ud-ud &>u.uw uu.c*i_
  t •      —  t*«. -?-i-» ^»/-*>--r\j^-r'a •f'fiH  into C2TOOS « 3_nC JLXlCl-LtlS
c3.dnn.uiii  Cciti  De incorpoi. a.L.CVJ.  .L.I.J.t-^ N^J_ ^ f >          ^^
   •     JT        f-amiTifli'^d  Qoils   Since trie  cirops wt*-^-*—«— — • —











land.
Chromium
                   Chromium is an elemental metal usually found as
                 CroOO-   The metal  is normally produced by
  educng tte oxide2wJth aluminum.   A significant proportion of -
 ?he cSomLm used is in the form  of compounds ~ch JB sodrum
 dichromate  (Na2Cr04) ,  and chromic acid (Cr03)   both are
 hexavalent  chromium compounds.
 inhibitors  for  closed water  circulation systems.
           in  its  various valence states, is hazardous to man.   It


                 sis'irs =
 mSrtons that show no effect in man
 prohibit determination, to  date.
                                                to be  so  low as to
                                  203

-------

  For the protection of human health from the toxic properties of
  chromium (except hexavalent chromium) ingested through waS? and
  contaminated aquatic organisms ,  the ambitnt water quality" crite-
  rion is 170 mg/1.   If contaminated aquatic organisms alone are
            Jxcl^dfnS the consumption 2f water, Sthe amb?en? water
                              ^ium ^ 3>443 mg/1.  The ambient
                              hexavalent chromium is recommended to
 Chromium  is not  destroyed  when treated by a POTW (althoueh   P
     a.f?in Stft&  ^y  ?hanse) »  and wil1 ei^er pass  through to ?he
      effu
-------
concentrations of total chromium of over 20,000 mg/kg  (dry basis)
have been observed.  Disposal of sludges containing very bj-gh'
concentrations of trivalent chromium can potentially cause prob-
lems in uncontrolled landfills.  Incineration  or  similar   • .
destructive oxidation processes, can produce hexavalent chromium
from lower valence states.  Hexavalent chromium is potentially
more toxic than trivalent chromium.  In cases where high rates  ot
chrome sludge application on land are used, distinct growth
inhibition and plant tissue uptake have been noted.

Pretreatment of discharges substantially reduces  the concentra-
tion of chromium in sludge.  In Buffalo, New York, pretreatment
of  electroplal-ine waste resulted in  a decrease  in chromium con-
cen?ratio£s in POTW sludge from  2,510 to  1,040  mg/kg.  A  similar
reduction occurred in Grand Rapids,  Michigan, POTW facilities
where the chromium concentration in  sludge decreased  from 11,000
to  2,700 mg/kg when pretreatment was made  a requirement.

Copper  (120).  Copper  is  a metallic  element that  sometimes is
l§Snf-fr^ras thS native metal, and is  also  found in minerals
such  as  cuprite  (Cu20), malechite  [CuC03.Cu(OH)2], azunte
 [2CuCOvCu(OH)2],  chalcopyrite (CuFeS2),  and bornite
 (CuqFeS/J.  Copper is  obtained from these ores  by smelting,
leaching and  electrolysis.   It  is  used in the  plating  electri-
cal,  plumbing,  and heating  equipment industries,  as well  as in
insecticides  and  fungicides.

Traces  of copper  are  found  in all  forms of plant and animal life,
and the metal  is  an  essential trace element for-nutrition.
 Copper  is not  considered  to  be a cumulative systemic poison for
humans  as  it  is  readily excreted by the body,.but it can cause
 symptoms of gastroenteritis,  with nausea and intestinal irrita-
 tions ,  as  relatively low dosages.   The limiting  factor in domes-
 tic water  supplies is taste.   To prevent this adverse organolep-
 tic effect  of copper in water, a criterion of 1 mg/JL has been
 established.

 The toxicity of copper to aquatic organisms varies significantly,
 not only with the species, but also with  the physical and chemi-
 cal characteristics of the water, including temperature', hard-
 nSss  turbidity, and carbon dioxide content.   In hard water, the
 ?Sxicity of copper salts may be reduced by the precipitation of
 copper carbonatS or other insoluble compounds.   The sulfates of
 copper and zinc, and of  copper and  calcium are synergistic  in
 their toxic effect on fish.

 Relatively high concentrations of copper  may be  tolerated by
 adult fish fo? short periods  of time; the critical effect of
 copper appears to be its higher toxicity  to young or  juvenile
 fish.  Concentrations of 0.02 to 0.03 mg/1 have  proved fatal  to
 some common fish  species.  In general  the salmonoids  are  very
 sensitive and the sunfishes  are less  sensitive to copper.
                                 205

-------
 The recommended criterion to protect  freshwater  aquatic  life  is
 0.0056 mg/1 as a 24-hour average, and 0.012 mg/1 maximum concen-
 tration at a hardness of 50 mg/1 CaCOa.  For total recoverable
 copper the criterion to protect freshwater aquatic life  is  0.0056
 mg/1 as a 24-hour average.

 Copper salts cause undesirable color  reactions in the food  indus-
 try and cause pitting when deposited  on some other metals such as
 aluminum and galvanized steel.  To control undesirable taste  and
 odor quality of ambient water due to  the organoleptic properties
 of copper, the estimated level is 1.0 mg/1 for total recoverable
 copper.                                    !~

 Irrigation water containing more than minute quantities  of copper
 can be detrimental to certain crops.  Copper appears in  all
 soils, and its concentration ranges from 10 to 80 ppm.   In soils,
 copper occurs in association with hydrous oxides of manganese and
 iron,  and also as soluble and insoluble complexes with organic
 matter.  Copper is essential to the life of plants, and  the
 normal range of concentration in plant tissue is from 5  to 20
 ppm.   Copper concentrations  in plants normally do not build up to
 high  levels  when toxicity occurs.   For example, the concentra-
 tions  of copper in snapbean  leaves and pods was less than 50 and
 20 mg/kg,  respectively,  under conditions of severe copper toxic-
 ity.   Even under conditions  of copper toxicity, most of the
 excess copper accumulates in the roots; very little is moved to
 the aerial part of the  plant.
                                            i
 Copper is  not destroyed  when treated by a POTW, and will  either
 pass through to the  POTW effluent  or be retained in the POTW
 sludge.   It  can interfere with the POTW treatment processes and
 can limit  the  usefulness of  municipal sludge.

 The influent  concentration of  copper to a POTW  has  been observed
 by the EPA to  range  from 0.01  to  1.97 mg/1,  with a median concen-
 tration of 0.12 mg/1.  The copper  that is  removed from the
 influent stream of a POTW is absorbed on the  sludge or appears in
 the sludge as  the hydroxide  of  the metal.   Bench scale pilot
 studies have  shown that  from about 25 percent to  75 percent  of
 the copper passing through the  activated sludge process remains
 in  solution  in  the final effluent.   Four-hour slug  dosages  of
 copper sulfate  in concentrations exceeding  50 mg/1  were reported
 to  have severe  effects on the removal  efficiency  of an unaccli-
 mated  system, with the system returning  to  normal  in  about  100
 hours.  Slug dosages  of  copper  in  the  form  of copper  cyanide were
 observed to have much more severe effects oh the  activated  sludge
 system, but the  total system returned  to normal in  24 hours.

 In  a recent study of  268 POTW facilities, the median  pass-through
was over 80 percent for  primary plants and  40 to  50 percent  for
 trickling filter, activated sludge, and  biological  treatment
                               206

-------
plants.  POTW effluent concentrations of^copper ranged  from 0.003
to 1.8 mg/1 (mean 0.126, standard deviation 0.242).

Copper which does not pass through the POTW will be retained  in
S!PSu5ge where it will build up ^ concentration   The  presence
of excessive levels of copper in sludge may limit its use on
cropland?  Sewage sludge contains up to 16,000 mg/kg of copper,
w?th 730 mg/kg Is the mean value.  These concentrations are
significantly greater than those normally  found in  soil,  which
usually rangl from 18 to 80 mg/kg.  Experimental data  indicate
that when dried  sludge  is spread over  tillable land  the  copper
tends  to remain  in place down to the depth of.the tillage, except
for copper which is taken up by plants grown  in the  soil.  Recent
investigation has shown that the extractable  copper  content  of
sludge-treated soil decreased with time, which suggests a rever-
sion of copper to less  soluble  forms was occurring.

Cyanide  (121).   Cyanides are among the most  toxic of pollutants
cgmmoniy-^o^sirved in  industrial wastewaters.   production of
cyanide into industrial processes  is usually by  dissolution of
potassium  cyanide  (KCN) or  sodium  cyanide  (NaCN)  in process
waters.  However, hydrogen  cyanide  (HCN)  formed  when the above
Tails  are  dissolved  in  water,  is probably  the most  acutely lethal
compound.

The relationship of  pH to hydrogen cyanide formation is very
important.   As  pH is  lowered to below 7,  more than 99 percent of
JS lyaSide  is  present  as  HCN and  less than  1 percent ^ as  cyanide
ions.   Thus,  at  neutral pH,  that of most living organisms, the
more  toxic form of cyanide  prevails.

 Cyanide ions  combine with numerous heavy metal ions to form  com-
plexes .  The complexes are in equilibrium with HCN.  Thus  the
Stability of the metal-cyanide complex and the pH determine  the
 concentration of HCN.  Stability of the metal-cyanide  anion  com-
 plexes is extremely variable.'  Those formed  with zinc, copper
 and cadmium are not stable - they rapidly dissociate   with pro-
 duction of HCN, in near neutral or acid waters.  Some  of^the com
 plexes are extremely stable.  Cobaltocyanide is very resistant  to
 acid  distillation in the laboratory.  Iron cyanide complexes are
 also  stable, but undergo photodecomposition  to give HCN  uPon
 exposure to sunlight.  Synergistic effects have been demonstrated
 for Se inSal cyanide complexes making zinc,,copper, and cadmium
 cyanides more toxic than an equal concentration of  sodium
 cyanide.

 The toxic mechanism of cyanide is essentially an inhibition of
 oxygen metabolism, i.e., rendering the tissues incapable of
 exchanging oxygen!  The cyanogen compounds  are tr^efln°n|^a^Ve
 protoplasmic poisons.  They arrest the activity of  all forms of
 animal life.  Cyanide  shows a very specific  type of toxic action.
                                 207

-------
                                             I
 It inhibits  the  cytochrome  oxidase system.   This system is the
 one which facilitates  electron  transfer from reduced metabolites
 to molecular oxygen.   The human body can convert cyanide to a
 non-toxic thiocyanate  and eliminate it.   However,  if the quantity
 ot cyanide ingested is  too  great at one time,  the  inhibition of
 oxygen utilization proves fatal before  the  detoxifying  reaction
 reduces the  cyanide concentration to a  safe level.

 Cyanides are  more toxic to  fish than to  lower  forms  of  aquatic
 organisms such as midge larvae,  crustaceans, and mussels.   Toxic-
 5 ^S-,      ^S a f"11^1011 of chemical form  and  concentration,  and
 is influenced by the rate of metabolism  (temperature),  the level
 of dissolved  oxygen, and pH.  In  laboratory studies  free  cyanide
 concentrations ranging from 0.05  to  0.14 mg/1 have been proven to
 S6,.^*  *° sensitive fish  species  including trout,  bluegill,  and
 fathead minnows.   Levels above  0.2 mg/1  are rapidly  fatal  to most
 tish species.  Long term sublethal  concentrations of cyanide as
 low as 0.01 mg/1  have been  shown  to  affect  the  ability of  fish to
 function normally,  e.g., reproduce,  grow, and swim.

 For the protection of human health  from  the toxic properties of
 cyanide ingested  through water and through contaminated aquatic
 £fSn  onnS)  ?he ambient water quality criterion  is determined to
 be 0.200 mg/1.

 Persistence  of cyanide in water is highly variable and depends
 upon  the chemical form of cyanide in the water, the concentration
 ot cyanide,  and the  nature of other constituents.  Cyanide may be
 destroyed by  strong  oxidizing agents such as permanganate and
 cnlonne.  Chlorine  is  commonly used to  oxidize strong cyanide
 solutions.   Carbon dioxide and  nitrogen  are  the products of com-
 plete  oxidation.  But  if the reaction is not complete, the very
 toxic  compound, cyanogen chloride, may remain in the  treatment
 system and subsequently be released to the environment.   Partial
 chlorination  may  occur  as  part  of a PQTW treatment, or during the
 disinfection  treatment  of  surface water  for  drinking  water prW-
 aration.                                                    r  ?

 Cyanides can  interfere with  treatment processes  in  a  POTW  or
 pass through  to ambient waters.   At  low  concentrations and with
 acclimated microflora, cyanide may be decomposed by microorga-
 nisms  in anaerobic and aerobic environments  or waste  treatment
 systems.  However, data  indicate that much of the cyanide intro-
 duced passes^through to the  POTW effluent.   The  mean  pass-through
 S£TIT *  ?}OS?-cal Plantswas  71 percent.   In  a recent  study of 41
 POTW facilities the effluent concentrations  ranged from  0.002 to
*SLm8/1 ^ea? =-2:518» standard  deviation = 15.6).   Cyanide also
enhances the toxicity of metals  commonly  found in POTW effluents  '
including the  toxic pollutants cadmium, zincj and copper.        '
                               208

-------
Data for Grand Rapids, Michigan, showed a significant decline  in
cyanide concentrations downstream from the POTW^after pretreat-
ment regulations were put in force.  Concentrations  fell  from
0.66 mg?l before, to 0.01 mg/1 after pretreatment was required.
            i
Lead (122).  Lead is a soft, malleable, ductile, blueish-gray
Seta-lTTc-ilement, usually obtained  from the mineral  galena  (lead
sulfide, PbS), anglesite  (lead sulfate, PbSO*), or cerussite
(lead carbonate, PbC03).  Because it is usually associated  with
minerals of zinc, silver, copper, gold, cadmium, antimony,  and
arsenic, special purification methods are frequently used before
and after extraction of the metal from the ore concentrate  by
smelting.

Lead is widely used for its corrosion resistance   sound and
vibration absorption, low melting point  (solders), and  relatively
high imperviousness to various  forms of radiation.   Small amounts
of copper,  antimony and other metals can be  alloyed  with lead  to
achieve greater  hardness, stiffness, or corrosion  resistance  than
is afforded by the pure metal.   Lead compounds  are used in  glazes
and paints.  About one third  of U.S. lead  consumption  goes  into
storage batteries.  About half  of U.S.  lead  consumption is  from
secondary  lead recovery.  U.S.  consumption  of lead is  in the
range of one million  tons annually.

Lead ingested by humans produces a  variety  of toxic  effects
including  impaired reproductive ability,  disturbances  in blood
chemistry",  neurological disorders,  kidney damage,  and  adverse
cardiovascular  effects.   Exposure  to  lead in the diet  results in
permanent  increase in lead  levels  in  the  body.   Most of the lead
entering  the body  eventually  becomes  localized in the  bones where
it  accumulates.  Lead is  a  carcinogen  or  cocarcinogen in some ^
species  of experimental  animals.  Lead is teratogenic in experi-
mental  animals.  Mutagenicity data are not available for lead.

The ambient water  quality criterion for lead is recommended to be
identical  to  the existng drinking water standard which is  0.050
mg/1.   Available data show that adverse effects on aquatic lite
occur  at concentrations  as  low as  7.5 x ICT^ mg/1 of total
recoverable lead as  a 24-hour average with a water hardness of 50
mg/1 as CaC03.

Lead is not destroyed in a POTW, but is passed through to  the
 effluent or retained in the POTW sludge; it can interfere  with
 POTW treatment processes and can limit the usefulness of POTW
 sludge for application to agricultural croplands.   Threshold  con-
 centration for inhibition of the activated sludge process  is  0.1
 mg/1,  and for the nitrification process is 0.5 mg/1.   In a study
 of 2l4 POTW facilities, median pass through values  were  over  80
 percent for primary plants and over 60 percent for  trickling
                                209

-------
 filter, activated sludge, and biological process plants.  Lead
 concentration in POTW effluents ranged from 0.003 to  1.8 mg/1
 (mean - 0.106 mg/1, standard deviation = 0.222).

 Application of lead-containing sludge to cropland should not lead
 to uptake by crops under most conditions because normally lead is
 strongly bound by soil.  However, under the unusual condition of
 low pH (less than 5.5) and low concentrations of labile phos-
 phorus, lead solubility is increased and plants can accumulate
 lead.                                      ,
                                           i
 Nickel (124).   Nickel is seldom found in nature as the pure ele-
 mental metal.   It is a relatively plentiful element and is widely
 distributed throughout the earth's crust.   It occurs in marine
 organisms and  is found in the oceans.  The chief commercial ores
 for nickel are pentlandite [(Fe,Ni)9Sg],  and a laterltic ore
 consisting of  hydrated nickel-iron-magnesium silicate.

 Nickel has many and varied uses.   It is used in alloys and as the
 pure metal.  Nickel salts are used for electroplating baths.

 The^toxicity of nickel to man is  thought  to be very low, and sys-
 temic  poisoning of human beings by nickel  or nickel salts is
 almost unknown.   In non-human mammals nickel acts to inhibit
 insulin release,  depress growth,  and reduce cholesterol.  A high
 incidence  of cancer of the lung and nose has been reported in
 humans engaged in the  refining of nickel.

 Nickel salts can  kill  fish at very low concentrations.  However,
 nickel has been  found  to be less  toxic to  some fish than copper,
 zinc,  and  iron.   Nickel  is present in coastal  and open ocean
 water  at concentrations  in the range of 0.0001 to 0.006 mg/1
 although the most common values are 0.002  to 0.003  mg/1.  Marine
 animals contain^up  to  0.4 mg/1  and marine  plants  contain up  to  3
 mg/1.   Higher  nickel concentrations have been  reported to cause
 reduction  in photosynthetic  activity of the  giant kelp.   A low
 concentration  was found  to kill oyster eggs.

 For  the protection  of  human  health based on  the  toxic  properties
 of nickel  ingested  through water  and through contaminated  aquatic
 organisms, the ambient water  criterion is  determined to  be 0.0134
 mg/1.   If contaminated aquatic organisms are consumed,  excluding
 consumption  of water,  the  ambient  water criterion is determined
 to be  0.100  mg/1.  Available  data  show that  adverse  effects  on
 aquatic life occur  for total  recoverable nickel  concentrations as
 low as 0.0071 mg/1 as  a  24-hour average.

 Nickel is not destroyed when  treated  in a POTW, but  will either
pass through to the POTW effluent  or  be retained  in  the  POTW
 sludge.  It  can interfere with POTW  treatment  processes  and  can
also limit the usefulness  of municipal  sludge.
                               210

-------
Nickel salts have caused inhibition of the biochemical  oxidation
of sewage in a POTW.  In a pilot plant, slug doses of nickel
significantly reduced normal treatment efficiencies  for a tew
hoSrs  but the plant acclimated itself somewhat  to the  slug dos-
aae and appeared to achieve normal treatment efficiencies ^ within
40 hours.  It has been reported that the  anaerobic digestion  pro-
cess is inhibited only by high concentrations  of nickel,  while a
low concentration of nickel inhibits the  nitrification  process.

The influent concentration of nickel to a POTW has been observed
by the EPA to range from 0.01 to 3.19 mg/1, with a median of  0. 33
me/1   In a study of 190 POTW facilities,  nickel pass-through was
e?eater than 90 percent for 82 percent of the  primary plants .
Median pass-through for trickling  filter,  activated  sludge  and
biological process plants was greater than 80  percent.   POTW
effluent concentrations ranged  from  0.002 to  40  mg/1 (mean -
0.410, standard, deviation = 3.279).

Nickel not passed through the POTW will be incorporated into  the
sludge.  In a recent two-year study  of eight  cities, four of  the
cities had median nickel concentrations  of over  350  mg/kg, and
two were over  1,000 mg/kg.  The  maximum nickel concentration
observed was  4,010 mg/kg.

Nickel  is  found  in  nearly  all  soils, plants,  and waters.  Nickel
has no known  essential  function in plants.  In soils, nickel
typically  is  found  in  the  range from 10  to 100 mg/kg.  Various
environemntal  exposures  to  nickel  appear  to correlate with _
increased  incidence of tumors  in man.   For example,  cancer in the
maxillary  antrum of snuff  users may result from using plant
materials  grown on  soil high in nickel.

Nickel  toxicity may develop in plants from application of sewage
sludge  on  acid soils.   Nickel  has caused reduction  of yields  for
a variety of crops  including oats, mustard, turnips, and  cabbage.
 In one  study nickel decreased the yields of oats significantly at
 100 mg/kg.

Whether nickel exerts a toxic effect on plants  depends on several
 soil factors,  the amount of nickel applied, and  the contents  ot
 other metals in the sludge.  Unlike copper and  zinc, which are
 more available from inorganic sources than from sludge,  nickel
 uptake by plants seems to be promoted by  the  presence  of the
 organic matter in sludge.   Soil treatments, such as liming,     ^
 reduce the solubility ^ of nickel.  Toxicity of nickel to  plants is
 enhanced in acidic soils.
Selenium (125).
element
                  Selenium  (chemical  symbol  Se)  is  a non-metallic
                  in several allotropic  forms.   Gray selenium,
                                             "
 element, e-x.jLsuj-i.ig  j-n o^v^j-^j- "••*-'	*	       -        .  -
 which has a metallic appearance,  is  the  stable  form at ordinary
 temperatures and  melts  at  220°C    e«i^4,,m-*a  * ^-.OT- mnmonent
                                  Selenium  is  a  major  component
                                211

-------
 of 38 minerals and a minor component of 37 others found in
 various parts of the world.  Most selenium is obtained as a
 by-product of precious metals recovery from electrolytic copper
 refinery slimes.  U.S. annual production at one time reached one
 million pounds.
                                            frii' », • ••'  "    ,   	

 Principal uses of selenium are in semi-conductors, pigments,
 decoloring of glass, zerography, and metallurgy.  It also is used
 to produce ruby glass used in signal lights.  Several selenium
 compounds are important oxidizing agents in!the synthesis of
 organic chemicals and drug products.

 While results of some studies suggest that selenium may be an
 essential element in human nutrition, the toxic effects of
 selenium in humans are well established.  Lassitude, loss of
 hair, discoloration and loss of fingernails are symptoms of
 selenium poisoning.  In a fatal case of ingestion of a larger
 dose of selenium acid, peripheral vascular collapse, pulmonary
 edema, and coma occurred.  Selenium produces mutagenic and tera-
 togenic effects,  but it has not been established as exhibiting
 carcinogenic activity.                     '

 For the protection of human health from the toxic properties of
 selenium ingested through water and through • contaminated aquatic
 organisms,  the ambient water criterion is determined to be 0.010
 mg/1, i.e.,  the  same as the drinking water standard.  Available
 data show that adverse effects on aquatic life occur at con-
 centrations  higher than that cited for human toxicity.

 Very few data are available regarding the behavior of selenium in
 a  POTW.   One EPA survey of 103 POTW facilities revealed one POTW
 using biological  treatment and having selenium in the influent.
 Influent concentration was 0.0025 mg/1,  effluent concentration
 was  0.0016 mg/1,  giving a removal of 37 percent.  It is not known
 to be inhibitory  to POTW processes.   In another study,  sludge
 from POTW facilities  in 16 cities was found to contain  from 1.8
 to 8.7 mg/kg selenium,  compared to 0.01  to 2 mg/kg in untreated
 soil.  ^These concentrations  of selenium in sludge present  a
 potential hazard  for  humans  or other  mammals eating crops  grown
 on soil  treated with  selenium-containing  sludge.

 Silver (126).  Silver is  a soft,  lustrous,  white metal  that is
 insoluble in water  and  alkali.   In nature,  silver is found  in the
 elemental state  (native  silver)  and combined in ores such as
 argentite (Ag£S), horn  silver  (AgCl),  proustite (Ag3AsS3),
 and pyrargyrite  (Ag3SbS3).   Silver is  used  extensively  in
 several  industries, among them electroplating.

Metallic  silver is  not  considered to  be toxic,  but most  of  its
 salts  are toxic to  a  large number of  organisms.   Upon ingestion
                               212

-------
by humans, many silver salts are absorbed in the circulatory  sys-
tem and deposited in various body tissues, resulting  in_general-
ized or sometimes localized gray pigmentation of the  skin  and
mucous membranes known as argyria.  There is no known method  for
removing silver from the tissues once  it is deposited,  and the
effect is cumulative.

Silver is recognized as a bactericide  and doses from  0.000001 to
0.0005 mg/1 have been reported as sufficient to sterilize  water.
The criterion for ambient water to protect human health from  the
toxic properties of silver ingested through water  and through
contaminated aquatic organisms is 0.010 mg/1.

The chronic toxic effects of silver on the aquatic environment
have not been given as much attention  as many other heavy  metals.
Data from existing literature support  the fact that silver is
very toxic to aquatic organisms.  Despite the fact that silver  is
nearly the most toxic of the heavy metals, there are  insufficient
data to adequately evaluate even the effects of hardness^on
silver toxicity.  There are no data available on the  toxicity of
different forms of silver.

There is no available literature on the  incidental removal of
silver by a POTW.  An incidental removal of about  50  percent  is
assumed as being representative.  This is the highest average
incidental removal of any metal for which data are available.
(Copper has been indicated to have a median incidental  removal
rate of 49 percent.)

Bioaccumulation and concentration of silver from  sewage sludge
has not been  studied to any great degree.  There  is some  indica-
tion that silver could be bioaccumulated  in mushrooms to  the
extent that there could be adverse physiological  effects  on
humans if they consumed large quantities  of mushrooms grown in
silver enriched soil.  The effect, however, would  tend  to  be
unpleasant rather than fatal.

There is  little summary data  available on the  quantity  of  silver
discharged to a POTW.  Presumably  there  would  be  a tendency to
limit its discharge  from  a manufacturing facility  because  of its
high  intrinsic value.

Thallium  (I27±.  Thallium (Tl)  is  a  soft,  silver-white, dense,
malleable metal.  Five major  minerals  contain  15  to 85 percent
thallium, but they  are not  of commercial importance because the
metal is  produced  in  sufficient  quantity as  a  by-product of lead-
zinc  smelting of  sulfide  ores.   Thallium melts  at 304 C.   U.S.
annual production of  thallium and  its  compounds  is estimated to
be 1,500  pounds.
                                213

-------
 Industrial uses of thallium include the manufacture of alloys,
 electronic devices and special glass.  Thallium catalysts are
 used for industrial organic syntheses.
 Acute thallium poisoning in humans has been widely described.
 Gastrointestinal pains and diarrhea are followed by abnormal
 sensation in the legs and arms, dizziness, and, later, loss of
 hair.   The central nervous system is also affected.  Somnolence,
 delerium or coma may occur.  Studies on the teratogenicity of
 thallium appear inconclusive; no studies on mutagenicity were
 found;  and no published reports on carcinogenicity of thallium
 were  found.'                               !	

 For the protection of human health from the toxic properties of
 thallium ingested through water and contaminated aquatic
 organisms,  the ambient water criterion is 0.004 mg/1.

 No reports  were found regarding the behavior of thallium in a
 POTW.   It will not be degraded, therefore it must pass through to
 the effluent  or be removed with the sludge.   However, since the
 sulfide (T1S) is very insoluble, if appreciable sulfide is
 present dissolved thallium in the influent to a POTW may be pre-
 cipitated into the sludge.   Subsequent use of sludge bearing
 thallium compounds as a soil amendment to crop bearing soils may
 result  in uptake of this element by food plants.  Several leafy
 garden  crops  (cabbage,  lettuce, leek,  and endive) exhibit rela-
 tively  higher concentrations of thallium than other foods such as
 meat.

 Zinc  (128).   Zinc occurs abundantly in the earth's crust, con-
 centrated in  ores.   It  is readily refined into the pure,  stable,
 silver-white  metal.   In addition to its  use  in alloys,  zinc is
 used as  a protective coating on steel.   It;is applied by hot dip-
 ing (i.e.,  dipping the  steel in molten zinc)  or by electroplat-
 ing-                                       ;
                                           l
 Zinc can  have an adverse effect on man and animals at high con-
 centrations.   Zinc  at concentrations in  excess of 5 mg/1  causes
 an undesirable taste which  persists through  conventional  treat-
 ment.    For  the  prevention of adverse effects  due to these organo-
 leptic  properties  of zinc,  5 mg/1 was  adopted for the ambient
water criterion.   Available  data show  that adverse effects  on
 aquatic  life  occur  at concentrations as  low  as 0.047 mg/1 as a
 24-hour average.

 Toxic  concentrations  of  zinc  compounds cause  adverse changes in
 the morphology  and physiology of fish.   Lethal concentrations  in
the range of  0.1 mg/1 have been reported.  Acutely toxic  concen- '
 trations  induce  cellular  breakdown  of  the  gills,  and possibly  the
clogging of the  gills with mucous.  Chronically  toxic concentra-
tions  of zinc  compounds  cause general  enfeeblement and widespread
                               214

-------
histological changes to many organs, but not to gills.  Abnormal
swimming behavior has been reported at 0.04 mg/1.  Growth and
maturation are retarded by zinc.  It has been observed that the
effects of zinc poisoning may not become apparent immediately, so
that fish removed from zinc-contaminated water may die as long as
48 hours'after removal.

In general, salmonoids are most sensitive to elemental zinc in
soft water: the rainbow trout is the most sensitive  in hard
waters.  A complex relationship exists between zinc  concentra-
tion, dissolved zinc concentration, pH, temperature,  and  calcium
and magnesium concentration.  Prediction of harmful  effects has
been less than reliable and controlled studies have  not been
extensively documented.
      '•~-. _v
The major concern with zinc compounds  in marine waters is not
with acute lethal effects, but  rather  with  the  long-term  sub-
lethal effects of the metallic  compounds and complexes.   Zinc
accumulates in some marine species, and marine  animals contain
zinc in the range of 6 to  1,500 mg/kg.  From^the  point of view  of
acute  lethal effects,  invertebrate  marine  animals seem to be  the
most sensitive organism tested.

Toxicities of zinc  in nutrient  solutions have been demonstrated
for a  number of plants.  A variety  of fresh water plants  tested
manifested harmful  symptoms at  concentrations of 0.030 to 21.b
me/1.   Zinc  sulfate has also  been  found  to  be  lethal to  many
plants  and  it could  impair agricultural  uses of the water.

Zinc is not  destroyed  when treated  by a  POTW, but will  either
pass through to  the POTW  effluent  or  be  retained in^the  POTW
sludge.   It  can  interfere  with treatment  processes in the POTW
and  can also  limit  the usefulness  of municipal  sludge.

In slue doses,  and  particularly in the presence of copper,  dis-
 solved zinc  can  interfere  with or  seriously disrupt the operation
of POTW biological  processes  by reducing overall removal effi-
ciencies,  largely as  a result of the toxicity of the metal to
biological organisms.   However, zinc solids in the form of
hydroxides or  sulfides do not appear to interfere with biological
 treatment processes,  on the basis  of available data.  Such solids
 accumulate in the sludge.

 The influent concentrations  of zinc to a POTW has been observed
 by the EPA to range from 0.017 to 3.91 mg/1, with a median con-
 centration of 0.33 mg/1.   Primary treatment is not efficient in
 removing zinc; however, the microbial floe of secondary treatment
 readily adsorbs zinc.

 In a study of 258 POTW facilities, the median pass-through values
 were 70 to 88 percent for primary plants,  50 to  60 percent for
                                215

-------
 trickling filter and biological process plants, and 30 to 40 per-
 cent for activated process plants.  POTW effluent concentrations
 of zinc ranged from 0.003 to 3.6 mg/1 (mean = 0.330, standard
 deviation = 0.464).
                                           i

 The zinc which does not pass through the POTW is retained in the
 sludge.  The presence of zinc in sludge may limit its use on
 cropland.  Sewage sludge contains 72 to over 30,000 mg/kg of
 zinc,  with 3,366 mg/kg as the mean value.  These concentrations
 are significantly greater than those normally found in soil,
 which range from 0 to 195 mg/kg, with 94 mg/kg being a common
 level.   Therefore, application of sewage sludge to soil will
 generally increase the concentration of zinc in the soil.  Zinc
 can be  toxic to plants, depending upon soil pH.   Lettuce, toma-
 toes,  turnips, mustard, kale, and beets  are especially sensitive
 to  zinc contamination.
Oil  and Grease.
tant parameter.
components  are:
Oil and grease are taken together as one pollu-
This is a conventional pollutant and some of its
      1.   Light  Hydrocarbons - These include light fuels such as
 fasoline,  kerosene,  and jet fuel,  and miscellaneous solvents used
 or  industrial  processing,  degreasing,  or cleaning purposes.  m1-~
presence  of  these  light hydrocarbons may make the removal of
other heavier oil  wastes more difficult.
                                             The
      2.  Heavy Hydrocarbons,  Fuels,  and Tars - These include the
crude oils, diesel  oils,  #6  fuel  oil,  residual oils, slop oils,
and in some cases,  asphalt and  road  tar.   j

      3.  Lubricants  and Cutting Fluids - These generally fall
into  two classes:   non-emulsifiable  oils such as  lubricating oils
and greases and emulsifiable  oils  such as  water soluble oils,
rolling oils, cutting  oils,  and drawing compounds.   Emulsifiable
oils  may contain fat,  soap,  or  various other additives.
                                           !
      4.  Vegetable  and Animal Fats and Oil's  - These  originate
primarily from processing of  foods and natural products.

These compounds can  settle or float  and may  exist as solids  or
liquids depending upon factors  such  as method of use,  production
process, and temperature of water.

Oil and grease even  in small  quantities cause troublesome taste
and odor problems.   Scum lines  from  these  agents are produced on
water treatment basin  walls and other  containers.  Fish  and  water
fowl are adversely affected by  oils  in their habitat.   Oil emul-
sions may adhere to  the gills of fish  causing suffocation, and
the flesh of fish is tainted when microorganisms that  were
exposed to waste oil are eaten.  Deposition  of oil in  the bottom
                               216

-------
sediments of water can serve to inhibit normal benthic growth.
Oil and grease exhibit an oxygen demand.

Many of the toxic organic pollutants will be found distributed
between the oil phase and the aqueous phase in industrial waste-
waters.  The presence of phenols, PCB's, PAH's, and  almost  any
other organic pollutant in the oil and grease make characteriza-
tion of this parameter almost impossible.  However,  all^of  these
other organics add to the objectionable nature of the oil and
grease.

Levels of oil and grease which are toxic to aquatic  organisms^
vary greatly, depending on the type  and the species  susceptibil-
ity.  However, it has been reported  that crude oil in concentra-
tions as low as 0.3 mg/1 is extremely toxic to freshwater fish.
It has been recommended that public  water  supply sources be
essentially free from oil and grease.

Oil and grease in quantities of  100  1/sq km show up  as  a  sheen on
the surface of a body of water.   The presence of oil slicks
decreases the aesthetic value of a waterway.

Oil and grease is compatible with a  POTW activated  sludge process
in limited quantity.  However, slug  loadings  or high concentra-
tions of oil and grease interfere with  biological  treatment
processes.  The oils coat surfaces and  solid  particles, prevent-
ing access of oxygen, and sealing in some  microorganisms.   Land
spreading of POTW sludge containing  oil  and grease uncontamrnated
by toxic pollutants  is not  expected  to  affect crops  grown on the
treated land, or animals eating  those  crops.

PH.  Although not a  specific pollutant,  pH is related to  the
acidity or alkalinity of a  wastewater  stream.   It  is not,  how-
ever,  a measure of either.   The  term pH is used  to describe the
hydrogen  ion  concentration  (or  activity) present  in a given solu-
tion.  Values  for pH range  from 0 to 14,  and  these numbers  are
the negative  logarithms  of  the  hydrogen ion concentrations.  A pH
of  7  indicates neutrality.   Solutions  with a  pH above 7 are alka-
line,  while  those  solutions with a pH below 7 are acidic.   The
relationship  of pH  and  acidity  and  alkalinity is  not necessarily
linear or  direct.   Knowledge of the  water  pH is  useful in deter-
mining necessary  measures  for  corrosion control,  sanitation, and
disinfection.   Its  value  is also necessary in the treatment of
 industrial wastewaters  to  determine  amounts of chemicals required
to remove  pollutants and to measure their effectiveness.   Removal
of pollutants,  especially  dissolved solids is affected by the pH
of the wastewater.

Waters with a pH below 6.0 are corrosive to water works struc-
 tures, distribution lines,  and household plumbing fixtures and
 can thus add constituents  to drinking water such as iron, copper,
                                217

-------
 zinc,  cadmium,  and lead.   The hydrogen ion concentration can
 affect the taste of the water, and at a low pH water tastes sour.
 The bactericidal effect of chlorine is weakened as the pH
 increases, and  it is advantageous to keep the pH close to 7.0.
 This is significant for providing safe drinking water.

 Extremes of pH  or rapid pH changes can exert stress conditions  or
 kill aquatic life outright.   Even moderate changes from accept-
 able criteria limits of pH are deleterious to some species.
                                           I
 The relative toxicity to  aquatic life of many materials is
 increased by changes in the  water pH.  For example, metallocya-
 nide complexes  can increase  a thousand-fold in toxicity with a
 drop of 1.5 pH  units.                      '

 Because of the  universal  nature of pH and its effect on water
 quality and treatment,  it is selected as a pollutant parameter
 for many industry categories.   A neutral pH range (approximately
 6 to 9)  is generally desired because either extreme beyond this
 range  has  a deleterious effect on receiving waters or the pollu-
 tant nature of  other wastewater constituents.

 Pretreatment for regulation  of pH is covered by the "General Pre-
 treatment  Regulations  for Existing and New Sources of Pollution,"
 40  CFR 403.5.   This  section  prohibits the discharge to a POTW of
 "pollutants  which will  cause corrosive structural damage to the
 POTW but  in no  case  discharges with pH lower than 5.0 unless the
 works  is  specially designed  to accommodate such discharges."

 Total  Suspended Solids  (TSS).   Suspended solids include both
 organic  and inorganic materials.   The inorganic compounds include
 sand,  silt,  and clay.   The organic fraction  includes  such materi-
 als  as  grease,  oil,  tar,  and animal and vegetable waste products.
 These  solids may settle out  rapidly,  and bottom deposits are
 often  a mixture of both organic and inorganic solids.   Solids may
be  suspended in water for a  time  and then settle to the bed of
 the  stream or lake.  These solids  discharged with man's wastes
may be  inert, slowly biodegradable materials,  or rapidly decom-
posable substances.  While in  suspension,  suspended solids
 increase the turbidity  of the  water,  reduce  light penetration,
and  impair  the  photosynthetic  activity of aquatic plants.

Suspended  solids  in water interfere with many industrial pro-
cesses and cause  foaming in  boilers  and  incrustations  on equip-
ment exposed to  such water,  especially as  the  temperature rises.
They are undesirable in process water  used in  the manufacture of
steel, in  the textile industry, in laundries,  in dyeing,  and in
cooling systems.

Solids in suspension are aesthetically displeasing.  When they
settle to  form  sludge deposits  on  the  stream or lake bed, they
                               218

-------
are often damaging to the life in the water.  Solids, when trans-
formed to sludge deposit, may do a variety of damaging things,
including blanketing the stream or lake bed and thereby destroy-
ing the living spaces for those benthic organisms that would
otherwise occxipy the habitat.  When of an organic nature, solids
use a portion or all of the dissolved oxygen available in the
area.  Organic materials also serve as a food source  for
sludge worms arid associated organisms.

Disregarding any toxic effect attributable to substances leached
out by water, suspended solids may kill fish and shellfish by
causing abrasive injuries and by clogging the gills and respira-
tory passages of various aquatic fauna.  Indirectly,  suspended
solids are inimical to aquatic life because they screen out
light, and they promote and maintain the development  of noxious
conditions through oxygen depletion.  This results  in the killing
of fish and fish food organisms.  Suspended solids  also reduce
the recreational value of the water.

Total suspended solids is a traditional pollutant which is com-
patible with a well-run POTW.  This pollutant with  the exception
of those components which are described elsewhere in  this  sec-
tion, e.g., heavy metal components, does not interfere with  the
operation of a POTW.  However, since a considerable portion  of
the  innocuous TSS may be inseparably bound  to the constituents
which do interfere with POTW operation, or  produce  unusable
sludge, or subsequently dissolve to produce unacceptable  POTW
effluent, TSS may be considered a toxic waste.

POLLUTANT SELECTION FOR COPPER FORMING WASTE STREAMS

The  pollutant selection procedure was performed for the  following
copper  forming waste streams to  select  those toxic  pollutants
that would be considered for establishing  regulations for  the
Copper  Forming Category:

     Cold Rolling Spent Lubricant
     Hot Rolling Spent Lubricant
     Drawing  Spent Lubricant
      Solution Heat Treatment  Contact  Cooling Water
     Extrusion Press Heat  Treatment  Contact Cooling Water
      Pickling Bath
     Pickling Rinse
     Alkaline Cleaning Bath
     Alkaline Cleaning Rinse
     Annealing  - Water
     Annealing  -  Oil
      Pickling Fume  Scrubber Water
                                219

-------
Pollutants Not Detected.   The  112  toxic pollutants  listed in
Table VI-1 were not  detected in  any  samples  from these wastewater
streams as reported  in  Tables  V-14 through V-25 (p.100 -175)-
therefore, they were not  selected  .for  consideration  in establish-
ing regulations.

Pollutants Detected  but Present  at Concentrations too  Small  to  be
Treated^The nine pollutants  listed in Table  VI-'1 were detected
in copper forming wastewater;  however,  they  were found at concen-
trations which were  not treatable.  Therefore,  they  were not
selected for consideration in  establishing regulations.

Pollutants Selected  for Regulation.  The  17  toxic pollutants
listed in Table VI-3 were those  not eliminated  from  consideration
for any of the reasons  listed  above; therefore,  each was selected
for consideration in establishing  regulations.

The maximum concentrations of  these toxic  pollutants which were
found in copper forming wastewaters are presented in Table VI-4.
                              220

-------
                          .Table VI-1

      POLLUTANTS NOT DETECTED IN COPPER FORMING WASTEWATER
 1.'  acenaphthene
 2.  acrolein
 3.  acrylonttrile
 5.  benzidine
 6.  carbon tetrachloride
 7.  chlorobenzene
 8.  1,2,4-trichlorobenzene
 9.  hexachlorobenzene
10.  1,2-dichloroethane
12.  hexachloroethane
13.  1,1-dichloroethane
14.  1,1,2-trichloroethane
15.  1,1,2,2-tetrachloroethane
16.  chloroethane
17.  DELETED
18.  bis(chloroethyl)ether
19.  2-chloroethyl vinyl ether
20.  2-chlor©naphthalene
21.  2,4,6-trichlorophenol
22.  p-chloro-m-cresol
24.  2-chlor©phenol
25.  1,2-dicb.lorobenzene
26.  1,3-dichlorobenzene
27.  1,4-dichlorobenzene
28.  3,3'-dichlorobenzidine
29.  1,1-dichloroethylene
30.  1,2-trans-dichloroethylene
31.  2,4-dichlorophenol
32.  1,2-dichloropropane
33.  1,3-dichloropropylene
34.  2,4-dimethylphenol
35.  2,4-dinitrotoluene
37.  1,2-diphenylhydrazine
39.   fluoranthene
40.  4-chlorophenyl phenyl ether
41.  4-bromophenyl phenyl ether
42.  bis(2-chloroisopropyl)ether
43.  bis(2-chloroethoxy)methane
45.  methyl  chloride  (chloromethane)
46.   methyl  bromide  (bromomethane)
47.  bromoform (tribromomethane)
48.   dichlorobromomethane
49.   DELETED
50.   DELETED
51.   chlorodibromomethane
                               221

-------
  52.
  53.
  54.
  56.
  57.
  58.
  59.
  60.
  61.
  63.
  64.
  65.
  66.
  67.
  68.
  69.
  70.
  71.
  72.
  73.
  74.
  75.
  76.
  77.
  79.
  80.
  82.
  83.
  84.
  85.
  88.
  89.
  90.
  91.
  92.
  93.
  94.
  95.
  96.
  97.
  98.
  99.
100.
101.
102.
                 Table VI-1  (Continued)

  POLLUTANTS NOT DETECTED IN COPPER FORMING  WASTEWATER


 hexachlorobutadiene
 hexachlorocyclopentadiene           j
 isophorone
 nitrobenzene
 2-nitrophenol                        .
 4-nitrophenol
 2,4-dinitrophenol
 4,6-dinitro-o-cresol
 N-nitrosodimethylamine
 N-nitrosodi-n-propylamine
 pentachlorophenol
 phenol
 bis(2-ethylhexyl)phthalate           .
 butyl benzyl phthalate
 di-n-butyl phthalate
 di-n-octyl phthalate
 diethyl
 dimethyl
phthalate
 phthalate
benzo(a)anthracene
benzo(a)pyrene
benzo(b)fluoranthene
benzo(k)fluoranthene
chrysene
acenaphthylene
benzo(ghi)perylene
fluorene
dibenzo(a,h)anthracene
indeno(1,2,3-c,d)pyrene
pyrene
tetrachloroethylene
vinyl chloride (chloroethylene)
aldrin
dieldrin
chlordane
4,4'-DDT
4,4'-DDE
4,4'-ODD
alpha-endosulfan
beta-endosulfan
endosulfan sulfate
endrin
endrin aldehyde
heptachlor
heptachlor epoxide
alpha-BHC
                               222

-------
                     Table VI-1 (Continued)

      POLLUTANTS NOT DETECTED IN COPPER FORMING WASTEWATER
103.
104.
105.
106.
107.
108.
109.
110.
111.
112.
113.
114.
115.
116.
117.
1 18 .
121.
123.
125.
126.
127.
129 .
beta-BHC
gamma- BHC
delta- BHC
PCB-1242
PCB-1254
PCB-1221
PCB-1232
PCB-1248
PCB-1260
PCB-1016
toxaphene
                 (a)
                 (a)
                 (a)
                 (a)
                 (b)
                 (b)
                 (b)
     arsenic
     asbestos
     beryllium
     cadmium
     cyanide
     mercury
     selenium
     silver
     thallium
     2,3,7 ,8-tetrachlorodibenzo-p-dioxin
(a)  (b)  Phenanthrene and anthracene are reported together since
        they are not physically distinguishable using approved
        analytical methods.
                               223

-------
                 Table VI-2

POLLUTANTS EXCLUDED FROM REGULATION BECAUSE
   THEY ARE PRESENT IN AMOUNTS TOO SMALL
         TO BE EFFECTIVELY TREATED
              Antimony

              Arsenic

              Beryllium

              Cadmium

              Cyanide

              Mercury

              Selenium

              Silver

              Thallium
                  224

-------
                            Table VI-3

               POLLUTANTS CONSIDERED FOR REGULATION
  4.   benzene
 11.   1,1,1-trichloroethane
 23.   chloroform
 36.   2,6-dinitrotoluene
 38.   ethylbenzene
 44.   methylene chloride
 5 5.   naphthalene
 62.   N-nitrosodiphenylamine
 7 8.   anthracene
 81.   phenanthrene
 86.   toluene
 87.   trichloroethylene
119.   chromium
120.   copper
122.   lead
124.   nickel
128.   zinc
                               225

-------
                            Table VI-4

            MAXIMUM CONCENTRATIONS OF TOXIC  POLLUTANTS
               FOUND IN COPPER FORMINQ WASTEWATERS
     Toxic Pollutant
4.
11.
23.
36.
38.
44.
55.
62.
78.
81.
86.
87.
119.
120.
122.
124.
128.
benzene
1,1,1 -tr ichloroethane
chloroform
2, 6-dinitrotoluene
e thy Ib enz ene
methylene chloride
naphthalene
N-ni t r o s od ipheny 1 amine
anthracene (a)
phenanthrene (a)
toluene
trichloroethylene
chromium
copper
lead
nickel
zinc
Maximum Concentration
      Observed	

        2.0 mg/1
        0.087 mg/1
        0.038 mg/1
       14.0 mg/1
        0.043 mg/1
        0.053 mg/1
        3.5 mg/1
       90 mg/1
       27 mg/1
       27 mg/1
        0.057 mg/1
        0.023 mg/1
      174 mg/1
   24,000 mg/1
      167 mg/1
      385 mg/1
   !45,000 mg/1
(a)   Phenanthrene and anthracene  are reported together since they
     are not physically distinguishable using approved analytical
     methods.
                                             lr"' "!'.' '',!': '.	.'!'"! :	:"'i ",'""!: K. 'Will	:-	[[,	,; >'. :'•.•»,	I	!!!'•,'(,' W™	I")'!
                               226

-------
                           SECTION VII

                 CONTROL AND TREATMENT TECHNOLOGY


This section describes the treatment techniques currently used or
available ?o remove or recover wastewater pollutants normally
generated b? the copper forming industrial point source^category.
Included are discussions of individual end-of-pipe treatment
technologiel and in -pi ant technologies.  These treatment technol-
ogies art widely used in many industrial categories and data and
information to support their effectiveness has been drawn from a
similarly wide range of sources and data bases.

KND-OF-PIPE TREATMENT TECHNOLOGIES

Individual recovery and treatment technologies are described
which are used or are suitable for use in treating wastewater
discharges from copper forming facilities.   Each description
?nc?udef a factional description and discussions of  application
and performance, advantages and limitations, operational Actors
 (reliability, maintainability, solid waste  aspects) ,- and demon-
stration status.  The treatment processes described  include both
technologies presently demonstrated within  the copper forming
category! and technologies  demonstrated  in  treatment  of similar
wastes  in other industries.

 Copper  forming wastewater  streams  characteristically contain
 significant  levels  of toxic inorganics.   Chromium,  copper,  lead,
SlcSl^Sd  zinc  are  found in copper  forming wastewater streams
 at substantial  concentrations.  These  toxic  inorganic pollutants
 constitute  the  most significant wastewater  pollutants in this
 category.
 In general, these pollutants are removed by oil removal
 min? emulsion breaking, and flotation), chemical precipitation
 aid sedimentation, or filtration.  Most of them may be effec-
 Svely removed by precipitation of metal hydroxides or carbonates
 utilizing the reaction with lime, sodium hydroxide, or sodium
 carbonate.  For some, improved removals are provided by the use
 of sodium sulfide or' ferrous sulfide to precipitate the pollu-
 tants as sulfide compounds with very low solubilities.

 Discussion of end -of -pipe treatment technologies is divided into
 three parts:  the major technologies; the effectiveness of major
 technologies; and minor end -of -pipe technologies.
                                227

-------
 MAJOR  TECHNOLOGIES
                                           i

 In Sections IX, X, XI,  and XII,  the rationale  for selecting
   ent  ^stems *:s  discussed.  The , individual  technologies  used
         system  are described here.   The major end-of-pipe  technol-
           i                 metals,  cyanide  precipitation,  granu-
         filtration  pressure  filtration  settling of suspended
     flionShi5i?8    ?Xl» che?ical emulsion  breaking,  and thermal
 emulsion breaking.  In practice, precipitation of metals and
 settling of the resulting precipitates is often a unified
 two-step operation.  Suspended solids originally present in raw
 wastewaters are not appreciably affected by  the precipitation
 operation and are removed with the precipitated metals in  the
 settling operations.  Settling operations can be evaluated
 independently of hydroxide or other chemical precipitation
 operations, but hydroxide and other chemical precipitation

 ?emovai°opera?ion"7 ^ SValuated in Combination with a solids

 Chemical Reduction of Chromium
     ;       °f the Procesg-  Reduction is a chemical reaction in
which electrons are transferred to the chemical being reduced
                                          emca   eng reuce
      the,che*ic*l initiating the transfer (the reducing agent).
 Sulfur dioxide,  sodium bisulfite,  sodium metabisulf itef and
 ferrous sulfate form strong reducing agents in aqueous solution
 and are often used in industrial waste treatment facilities for
 £oL~I:dUCt1?? °f hexavajent chromium to the trivalent form.  The
  ?3J  iS  allows removal of chromium from solution in conjunction
 with other metallic salts by alkaline precipitation.   Hexavalent
 chromium is not  precipitated as the hydroxide.         "exavaient

 Gaseous sulfur dioxide is a widely used reducing agent and pro-
 vides  a good example of the chemical reduction  process.   Reduc-
 fnSJiS8^ Ot5er.^a§ents is chemically similar.   The reactions
 involved may be  illustrated as  follows:
          3S02
                   2H2Cr04
                                         + 5H20
The above reactions are  favored by  low pH.  A pH  of  from 2  to  3
is normal for situations requiring  complete reduction.  At  pH
levels above 5, the reduction rate  is slow.  Oxidizing agents
such as dissolved oxygen and ferric iron interfere with the
reduction process by consuming the  reducing agent.

A typical treatment consists of 45 minutes retention in a
reaction tank.  The reaction tank has an electronic recorder-
controller device to control process conditions with respect to
                               228

-------
pH and oxidation-reduction potential (ORP).  Gaseous sulfur
dioxide is metered to the reaction tank to maintain the ORP
within the range of 250 to 300 millivolts.  Sulfuric acid is
added to maintain a pH level of from 1.8 to 2.0.  The reaction
tank is equipped with a propeller agitator designed to provide
approximately one turnover per minute.  Figure VII-1 shows a
continuous chromium reduction system.

Application and Performance.  Chromium reduction is used in
copper forming for treating pickling baths and pickling rinses.
Cooling tower blowdown may also contain chromium as a biocide^in
waste streams.  A study of an operational waste treatment facil-
ity chemically reducing hexavalent chromium has shown that a 99.7
percent reduction efficiency is easily achieved.  Reduction fol-
lowed by chemical precipitation can achieve final concentrations
of 0.05 mg/1, and concentrations of 0.01 mg/1 are considered to
be attainable by properly maintained and operated equipment.

Advantages and Limitations.  The major advantage^of^chemical
reduction to reduce hexavalent chromium is that it is a fully
proven technology based on many years of experience.  Operation
at ambient conditions results in low energy consumption, and the
process, especially when using sulfur dioxide,  is well suited  to
automatic control.  Furthermore, the equipment  is readily obtain-
able  from many  suppliers, and operation  is straightforward.

One  limitation  of chemical reduction  of hexavalent  chromium is
that  for high concentrations of chromium,  the  cost  of treatment
chemicals may be prohibitive.  When  this  situation  occurs, other
treatment techniques  are likely to be more economical.  Chemical
interference by oxidizing agents  is  possible  in the treatment  of
mixed wastesi and the treatment itself may introduce pollutants
if not properly controlled. - Storage  and  handling of  sulfur
dioxide  is  somewhat hazardous.

Operational Factors.  Reliability:  Maintenance consists  of
periodic removal of  sludge,  the  frequency of  which  is  a function
of the input  concentrations  of detrimental constituents.

Solid Waste Aspects:   Pretreatment  to eliminate substances which
will interfere  with the process  may  often be  necessary.   T^is^
process  produces trivalent  chromium which can be  controlled  by
 further  treatment.   There  may, however,  be small  amounts  of
 sludge  collected due to minor  shifts in the  solubility of the
 contaminants.   This  sludge  can be processed by the main sludge
 treatment equipment.
                                229

-------
 Demonstration Status.  The reduction of chromium waste by sulfur
 dioxide or sodium bisulfite is a classic process and is used by
 numerous plants which have hexavalent chromium compounds in
 wastewaters from operations such as electroplating and coil coat-
 ing.  Eight copper forming plants report the use of chromium
 reduction to treat pickling wastewaters.  :

 Chemical Precipitation

 Dissolved toxic metal ions and certain anions may be chemically
 precipitated for removal by physical means such as sedimentation
 filtration, or centrifugation.  Several reagents are commonly
 used to effect this precipitation.

      1.  Alkaline compounds such as lime or sodium hydroxide may
          be used to precipitate many toxic metal ions as metal
          hydroxides.   Lime also may precipitate phosphates as
          insoluble calcium phosphate and fluorides as calcium
          fluoride,

          Both "soluble" sulfides such as hydrogen sulfide or
          sodium sulfide and "insoluble" sulfides  such as ferrous
          sulfide may  be used to precipitate many  heavy metal ions
          as insoluble metal sulfides.

          Ferrous sulfate,  zinc sulfate,  or both (as  is  required)
          may be used  to precipitate cyanide as  a  ferro or zinc
          ferricyanide complex.

          Carbonate  precipitates  may be used to  remove  metals
          either by  direct  precipitation  using a carbonate
          reagent such as calcium carbonate  or by  converting
          hydroxides into carbonates  using  carbon  dioxide.

These  treatment  chemicals  may  be  added to  a flash mixer or rapid
mix tank, to a presettling tank,  or  directly  to a  clarifier  or
?thfri settling  device-  Because  metal hydroxides  tend  to  be  col-
loidal  in nature, coagulating  agents may also be  added  to facili-
tate settling.   After the  solids  have been  removed,  final pH
adjustment may be required to reduce the high pH  created  by  the
alkaline  treatment  chemicals.
                                           i

Chemical precipitation as  a mechanism for removing metals from
wastewater is a  complex process of at least two steps - precipi-
tation  of the unwanted metals and removal of  the precipitate.
Some small amount of  metal will remain dissolved in the waste-
water after complete  precipitation.  The amount of residual
dissolved metal depends on the treatment chemicals used and
related factors.  The effectiveness of this method of removing
any specific metal depends on the fraction ;of the specific metal
2.
3.
4.
                                           1	 - >	
                              230

-------
in the raw waste (and hence in the precipitate) and^the effec-
tiveness of suspended solids removal.  In specific  instances, *
sacrificial ion such as iron or aluminum may be added  to  aid  in
the precipitation process and reduce the fraction of a specific
metal in the precipitate.

Application and Performance.  Chemical precipitation is used  in
copper forming for precipitation of dissolved  metals.  It can be
used to remove metal ions such as antimony, arsenic, beryllium,
cadmium, chromium, cobalt, copper, iron, lead, manganese,
mercury, molybdenum, tin, and zinc.  The process  is also
applicable to any substance that can be transformed into  an
insoluble form such as  fluorides, phosphates   soaps,  sulfides
and others.  Because it is simple and  effective,  chemical precip-
itation is extensively  used for  industrial  waste  treatment.

The performance of chemical precipitation  depends on several
variables.  The most important  factors affecting  precipitation
effectiveness are:

      1.  Maintenance of an  alklaine  pH throughout the
         precipitation  reaction  and  subsequent settling;

      2.  Addition of a  sufficient  excess  of treatment ions to
         drive  the precipitation reaqtion to completion;

      3.  Addition of  an adequate supply of sacrificial ions
          (such  as  iron  or aluminum)  to ensure precipitation and
         removal  of  specific  target,  ions; and

      4.  Effective  removal of precipitated solids  (see
         appropriate  technologies discussed under  Solids
         Removal").

 Control of pH.   Irrespective of the solids removal technology
 employed,  proper control of pH is absolutely essential for favor-
 able performance of precipitation-sedimentation technologies.
 This is clearly illustrated by solubility curves for  selected
 metals hydroxides and sulfides shown  in Figure VII-2, and  by
 plotting effluent zinc concentrations against pH as shown  in
 Figure VII-3.  Figure VII-3 was obtained from Development  Docu-
  ent for the Proposed Effluent Limitations Guidelines and  New
Source Performance Standards foi
Metals Manufacturin
                      .^^^~~	the Zinc Segment  of
                      Point Source Category^U.S.E.P.A.,
Nonferrous
   "ER
 Metals FianuEacLurj-uK JTKJ.I.IL. u^m.»-^ ^^.^^f,^^j,  ~.~-	   ,
 440/1-74/033, November, 1974.Figure VII-3  was  plotted from the
 sampling data from several facilities with metal finishing
 operations.  It is partially  illustrated  by  data obtained from
 three consecutive days of sampling  at one metal  processing plant
 (47432) as displayed in Table VII-1.  Flow through this system is
 approximately 49,263 1/hr  (13,000 gal/hr).
                                231

-------
This treatment  system uses  lime  precipitation  (pH  adjustment)
followed by coagulant addition and  sedimentation.  Samples were
taken before  (in) and after (out) the  treatment  system.  The best
treatment for removal of copper  and zinc was achieved on day one,
when the pH was maintained  at a  satisfactory level.  The poorest
treatment was found on the  second 'day, when the  pH slipped to  an
unacceptably  low level and  intermediate values were  achieved on
the third day, when pH values were  less than desirable but in
between the first and second days.

Sodium hydroxide is used by one  facility  (plant  439) for pH
adjustment and  chemical precipitation, followed  by settling
(sedimentation  and a polishing lagoon) of;precipitated solids.
Samples were, taken prior to caustic addition and following the
polishing lagoon.  Flow through  the system is approximately
22,700 1/hr (6,000 gal/hr).  Metals removal data for this system
are presented in Table VII-2.

These data indicate that the system was operated efficiently.
Effluent pH was controlled  within the  range of 8.6 to 9.3, and
while raw waste loadings were not unusually high,  most toxic
metals were removed to very low  concentrations.

Lime and sodium hydroxide are sometimes used to  precipitate
metals.  Data developed from plant  40063, a facility with a
metal-bearing wastewater, exemplify efficient operation of a
chemical precipitation and  settling system.  Table VXI-3 shows
sampling data from this system,  which uses lime  and  sodium
hydroxide for pH adjustment, chemical  precipitation, polyelec-
trolyte flocculant addition, and sedimentation.  Samples were
taken of the raw waste influent  to  the system and  of the
clarifier effluent.  Flow through the  system is  approximately
19,000 1/hr (5,000 gal/hr).

At this plant, effluent TSS levels  were below 15mg/1 on each
day, despite average raw waste TSS  concentrationsof over 3,500
mg/1.  Effluent pH was maintained at approximately 8, lime addi-
tion was sufficient to precipitate  the dissolved metal ions, and
the flocculant addition and clarifier  retention  served to remove
effectively the precipitated solids.

Sulfide precipitation is sometimes  used to precipitate metals
resulting in improved metals removals.  Most metal sxilfides are
less soluble than hydroxides and the precipitates  are frequently
more effectively removed from water.  Solubilities for selected
metal hydroxide, carbonate, and  sulfide precipitates are shown in
Table VII-4 (Source:  Lange's Handbook of Chemistry).  Sulfide
precipitation is particularly effective ia removing specific
metals such as silver and mercury.   Sampling data  from three
industrial plants using sulfide  precipitation appear in Table
VII-5.  The data were obtained from three sources:
                              ,232

-------
     1.  Summary Report, Control and Treatment Technology for
         the Metal Finishing Industry:  Sulfide Precipitation,
         USEPA, EPA No. 625/8/80-003, 1979.:

     2.  Industry Finishing, Vol. 35, No. 11, November/ 1979.

     3.  Electroplating sampling data from plant 27045.

In all cases except iron, effluent concentrations are below 0.1
mg/1 and in many cases below 0.04 mg/1 for the three plants
studied.

Sampling data  from several  chlorine-caustic manufacturing plants
using  sulfide  precipitation demonstrate effluent mercury concen-
trations varying between 0.009 and 0.03 mg/1.  As shown in Figure
VII-2, the solubilities of PbS and Ag£S are lower at alkaline
pH levels than either  the corresponding hydroxides or  other  sul-
fide compounds.  This  implies that removal performance for lead
and silver sulfides should  be comparable  to or better  than that
for the heavy  metal hydroxides.  Bench scale tests on  several
types  of metal finishing and manufacturing wastewater  indicate
that metals removal to  levels of less than 0.05 mg/1 and in  some
cases  less than 0.01 mg/1 are common  in  systems using  sulfide
precipitation  followed by clarification.   Some of the  bench  scale
data,  particularly  in  the case  of  lead,  do not support such  low
effluent concentrations.  However,  lead  is consistently removed
to very  low  levels  (less than 0.02  mg/1)  in  systems using
hydroxide and  carbonate precipitation and sedimentation.

Of particular  interest is the ability of sulfide  to precipitate
hexavalent  chromium (Cr+6)  without prior reduction to  the  tri-
valent state as  is  required in  the hydroxide  process.  When  fer-
rous  sulfide is  used  as the precipitant,  iron and sulfide  act as
reducing agents  for the hexavalent chromium  according  to the
reaction:
      Gr03 + FeS  + 3H20
Fe(OH)3 + Cr(OH)3 + S
 The sludge produced in this reaction consists mainly of ferric
 hydroxides, chromic hydroxides,  and various metallic sulfides.
 Some excess hydroxyl ions are generated in this process, possibly
 requiring a downward readjustment of pH.

 Based on the available data, Table VII-6  shows the minimum relia-
 bly attainable effluent concentrations for sulfide precipitation-
 sedimentation systems.  These values are  used to calculate
 performance predictions of sulfide precipitation-sedimentation
 systems.  Table VII-6 is based on two reports:
                                233

-------
      1.   Summary Report,  Control and Treatment Technology  for  the
          Metal Finishing  Industry:   Sulfide Precipitation, USEPA.
          EPA No.  625/8/80-003,  1979.       '.	

      2.   Addendum to  Development Document  for Effluent  Limita-
          tions Guidelines and New Source Performance  Standards,
          Major Inorganic  Products Segment  of Inorganics Point
          Source Category, USEPA..  EPA Contract No7  EPA/68-01-
          3281  (Task 7), June, 1978.

Carbonate precipitation is sometimes  used  to precipitate metals,
especially where  precipitated metals  values are to  be recovered.
The  solubility of most metal  carbonates is intermediate between
hydroxide and  sulfide solubilities;  in addition,  carbonates  form
easily  filtered precipitates.

Carbonate ions appear to  be particularly useful in  precipitating
lead  and  antimony.  Sodium carbonate  has been observed  being
added at  treatment to improve lead precipitation and  removal in
some  industrial plants.   The  lead hydroxide and lead  carbonate
solubility curves displayed in  Figure VII-4 ("Heavy Metals
Removal," by Kenneth  Lanovette,  Chemical Engineering/Deskbook
Issue, Oct.  17, 1977) explain this phenomenon.
                                           i
Co-precipitation  with Iron - The presence  of substantial quanti-
ties  of iron in metal-bearing wastewaters  before  treatment has
been  shown to  improve the removal of  toxic metals.  In  some  cases
this  iron is an integral  part of the  industrial wastewater;  in
other cases  iron  is deliberately added as  a preliminary  or first
step  of treatment.  The iron  functions to  improve toxic metal
removal by three  mechanisms:  the iron co-precipitates with  toxic
metals forming a  stable precipitate which  desolubilizes the  toxic
metal; the iron improves  the  settleability of the precipitate;
and the large  amount  of iron reduces  the fraction of  toxic metal
in the precipitate.   Co-precipitation with iron has been prac-
ticed for many years  incidentally when iron was a substantial
constituent  of raw wastewater and intentionally when  iron salts
were  added as  a coagulant  aid.  Aluminum or mixed iron-aluminum
salts also have been  used.

Co-precipitation  using large amounts  of ferrous  iron  salts is
known as  ferrite  co-precipitation because  magnetic  iron oxide or
ferrite is formed.  The addition of ferrous  salts (sulfate)  is
followed  by alkali precipitation and  air oxidation.   The resul-
tant precipitate  is easily removed by  filtration and may be
removed magnetically.   Data illustrating the performance of
ferrite co-precipitation  is shown in Table VII-7.  The data  are
from:
     1.
Sources and Treatment of Wastewater in the Nonferrous
Metals Industry, USEPA, EPA No. 600/2-80-074. 1980.
                               234

-------
Advantages and Limitations

Chemical precipitation has proven to be an effective technique
for removing many pollutants from industrial wastewater.  It_
operates at ambient conditions and  is well suited to automatic
control.  The use of chemical precipitation may be  limited
because of interference by chelating agents, because of  possible
chemical interference of mixed wastewaters and treatment^chemi-
cals  or because of the potentially hazardous situation  involved
with the storage and handling of those chemicals.   Lime  is usu-
ally added as a slurry when used in hydroxide precipitation.  Tne
slurry must be kept well mixed and  the addition lines  periodi-
cally checked to prevent blocking of  the  lines, which  may  result
from a buildup of solids. Also, hydroxide precipitation  usually
makes recovery of the precipitated  metals difficult, because of
the heterogeneous nature of most hydroxide  sludges.

The major advantage of the sulfide  precipitation  process is  that
the extremely low solubility  of  most  metal  sulfides promotes very
high metal removal efficiencies; the  sulfide  process  also  has the
ability  to remove chromates  and  dichromates without preliminary
reduction of the  chromium  to  its trivalent  state.   In addition,
sulfide  can precipitate  metals  completed with most complexing
aaents.  The. process  demands  care;  however,  in  maintaining the pti
of the  solution  at  approximately 10 in order  to prevent the gen-
eration of toxic  hydrogen  sulfide  gas.   For this  reason, ventila-
tion  o£ the  treatment tanks  may  be  a necessary precaution in most
installations.   The use  of insoluble sulfides reduces the problem
of hydrogen  sulfide  evolution.   As  with hydroxide precipitation,
excess  sulfide  ion  must  be present  to drive the precipitation
 reaction to  completion.   Since the sulfide ion itself is toxic,
 sulfide addition must be carefully controlled to maximize heavy
 metals  precipitation with a minimum of excess sulfide to avoid
 the necessity of post treatment.  At very high excess sulfiae  _
 levels  and high pH,  soluble mercury-sulfide compounds may aiso oe
 formed.  Where excess sulfide is present, aeration of the efflu-
 ent stream can aid in oxidizing residual sulfide to the less
 harmful sodium sulfate (Na2S04). The cost of sulfide pre.ca.p-
 itants is high in comparison with  hydroxide precipitants, and
 disposal of metallic sulfide sludges may pose problems.  An
 essential element in effective sulfide precipitation  is the
 removal of precipitated solids from the wastewater and  proper
 disposal in an appropriate site.   Sulfide precipitation will also
 generate a higher volume of sludge than hydroxide  precipitation,
 resulting in higher disposal and dewatering  costs.  This ^ is
 especially true when ferrous sulf5.de is  used as  the precipitanu.

 Sulfide precipitation may be used  as a polishing treatment  after
 nydroxid! precipitation-sedimentation.   This treatment  configura-
 tion may provide the better treatment effectiveness of  sulfide
                                 235

-------
  precipitation while  minimizing the variability caused by changes
  in  raw waste  and  reducing  the  amount  of sulfide precipitant
  required.                                             r
           -vn              Alkali*e chemical precipita-
highly reliable, although proper monitoring and control
       Sulfide  alitation S
                                                         con
                Sulfide Palpitation Systems provide similar
 tion

 Pliability

 Maintainability:  The major maintenance needs involve periodic
 upkeep of monitoring equipment, automatic  feeding equipment
 mixing equipment, and other hardware.  Removal of accumulated
 sludge is necessary for efficient operation of precipitation-
 sedimentation systems.

 Solid Waste Aspects:  Solids which precipitate out are removed in
                        8t8p'  Ultimate1^  these "ollds require

 Demonstration Status.   Chemical precipitation of metal hydroxides
 is a classic waste treatment technology used by most industrial
 ?!££« treat*ent systems.   Chemical precipitation of metals in the
 carbonate form alone has  been found to be  feasible and is commer-
 cially used to permit  metals recovery and water reuse.   Full
 n™^00^6^1?} sulfide  Precipitation units are in operation at
 numerous  installations.   As noted earlier,  sedimentation to
 ff??r PreciPitates  Js discussed separately.   Chemical precipi-
 tation is currently  demonstrated at  36 copper forming plants.

 Cyanide Precipitation                       ',

 Cyanide precipitation, although a  method  for  treating cyanide in
  ^thr!^  d^S.n?t  destr°y  ^anide.  The cyanide  is  retained
    the sludge that is  formed.   Reports  indicate  that  during expo-
                  th\?yanide complexes  can  break  down and for?
 mo          v    r th:L! reason  the sludge from this treatment
 method must be disposed of carefully.
»       **? b? P^^Pitated and settled out of wastewaters by the
addition of zinc sulfate or ferrous sulfate.  In the presencJ of
                                         ae.   n  te presenc   of
«JS?£.?Cyan£ de.wl11 nf2rm  extremely  stable cyanide  complexes.  The
addition of zinc sulfate or ferrous sulfate  forms zinc ferrocya-
nide or ferro and ferricyanide  complexes.
™oiron     PreciPitated cyanide requires that the PH
must be kept at 9.0 and an appropriate detention^ time be main-
tamed.  A study has shown that the formation of the complex is
IonLd?Pe?dent °n PH- ,At PH s of 8 and 10 the residual cyanidl
concentrations measured are twice those of the same reaction car-
ried out at a>PH of 9.  Removal efficiencies also depend heavily
on the retention time allowed.  The formation of the complexes
                               236

-------
takes place rather slowly.  Depending upon the excess amount of
zinc sulfate or ferrous sulfate added,-at least a 30 minute
retention time should be allowed for the formation of the cyanide
complex before continuing on to the clarification stage.

One experiment with an initial concentration of 10 mg/1 of cya-
nide showed that 98 percent of the cyanide was complexed 10
minutes after the addition of ferrous sulfate at twice the theo-
retical amount necessary.  Interference from other metal ions,
such as cadmium, might result in the need for longer retention
times.

Table VII-8 presents data from three  coil coating plants.  Plant
1057 also does aluminum  forming.  A fourth plant was visited^for
the purpose of observing plant testing of'the cyanide precipita-
tion system.  Specific data from this facility are not  included
because:   (1) the pH was usually well below the optimum level of
90; (2) the historical  treatment data were not obtained using
the  standard  cyanide analysis procedure; and  (3) matched_input-
output  data were not made available by the plant.  Scanning  the
available  data  indicates that the raw waste CN level was in  the
range of 25.0; the pH  7.5; and treated CN level was  from O.I  to
0.2.

The  concentrations are those  of  the  stream  entering  and leaving
the  treatment system.  Plant  1057 allowed a 27 minute  retention,
time for  the  formation of the complex.   The retention  time  for_
the  other  plants  is  not  known.   The  data suggest  that  over  a wide
ranee  of  cyanide  concentration  in the raw waste,  the concentra-
tion of cyanide can  be reduced  in the effluent stream  to under
0.15 mg/1.

Application and Performance.   Cyanide precipitation can be used
when cyanide  destruction is  not feasible because of the presence
 of cyanide complexes which are difficult to destroy.   Effluent
 concentrations of cyanide well  below 0.15 mg/1 are possible.

 Advantages and Limitations.   Cyanide precipitation is  an inexpen-
 sive method of treating cyanide.  Problems  may occur when metal
 ions interfere with the formation of the complexes.

 Demonstration Status.   Although no plants currently_use cyanide
 precipitation to treat  copper forming wastewaters, it  is used in
 at least six coil coating plants.

 Granular Bed Filtration

 Filtration occurs in nature as the surface ground waters are
 cleansed by  sand.  Silica sand, anthracite coal, and garnet  are
                                237

-------
 common filter media used in water treatment plants.  These  are
 usually supported by gravel.  The media may be used singly  or in
 combination.  The multi-media filters may be arranged to maintain
 relatively distinct layers by virtue of balancing the forces of
 gravity?( flow, and buoyancy on the individual particles.  This is
 accomplished by selecting appropriate filter flow rates  (epm/sq-
 ft), media grain size, and density.

 Granular bed filters may be classified in terms of filtration
 rate, filter media, flow pattern, or method of pressxirization.
 Traditional rate classifications are slow sand, rapid sand, and
 high rate mixed media.  In the slow sand filter, flux or
 hydraulic loading is relatively low, and removal of collected
 solids to clean the filter is therefore relatively infrequent.
 The filter is often cleaned by scraping off the inlet face  (top)
 of the sand bed.   In the higher rate filters,  cleaning is fre-
 quent and is accomplished by a periodic backwash, opposite  to the
 direction of normal flow.

 A"filter  may use  a single medium such as sand or diatomaceous
 earth (Figure VII-5a), but dual (Figure VII-5d) and mixed (multi-
 Pil< media (Figure Vll-Se)  filters  allow higher flow rates  and
 efficiencies.  'The dual media filter usually consists of a fine
 bed of sand under a coarser bed of  anthracite  coal.   The coarse
 coal removes most of the influent solids,  while the fine sand
 performs  a polishing function.   At  the  end of  the backwash,  the
 fine sand  settles to the bottom because it is  denser than the
 coal,  and  the  filter is ready for normal operation.   The mixed
 media filter operates  on the same principle, with the finer
 denser media at the bottom  and  the  coarser,  less dense  media at
 the top.   The  usual arrangement  is  garnet  at  the bottom (outlet
 end;  of the bed,  sand  in the  middle,  and anthracite  coal at  the
 top.   Some  mixing of these  layers occurs  and  is,  in  fact,
 desirable.

 The  flow pattern  is  usually  top-to-bottom, but  other  patterns  are
 sometimes used.   Upflow filters  (Figure VIl-5b)  are  sometimes
 used,  and in a horizontal filter  the  flow  is horizontal.  In a
 biflow filter  (Figure VII-5c),  the  influent enters both  the  top
 and  the bottom and  exits laterally.   The advantage of an upflow
 filter is that with an  upflow backwash  the particles  of  a single
 filter medium are distributed and maintained in  the desired
 coarse-to-fine (bottom-to-top) arrangement.  The  disadvantage  is
 that the bed tends  to become  fluidized, which lowers filtration
 efficiency.  The biflow design is an  attempt to  overcome  this
problem.
                               238

-------
The classic granular bed filter operates by gravity flow; how-
ever, pressure filters are fairly widely used.  They permit
higher solids loadings before cleaning and are advantageous when
the filter effluent must be pressurized for further downstream
treatment.  In addition, pressure filter systems are often less
costly for low to moderate flow rates.

Figure VII-6 depicts a high rate, dual media, gravity downflow
granular bed filter, with self-stored backwash.  Both filtrate
and backwash are piped around the bed in an arrangement  that per-
mits gravity upflow of the backwash, with the stored filtrate
serving as backwash.  Addition of the indicated coagulant and
polyelectrolyte usually results in  a substantial improvement in
filter performance.

Auxiliary filter cleaning is sometimes employed in  the upper few
inches of filter beds.  This is conventionally referred  to as
surface wash and is accomplished by water jets just below the
surface of the expanded bed during  the backwash cycle.   These
jets enhance the scouring action in the bed by increasing the
agitation.

An important  feature  for  successful filtration and  backwashing  is
the underdrain.  This  is  the support  structure for  tne bed.  The
underdrain provides an area  for  collection  of the  filtered water
without clogging from either the filtered solids or the  media
grains.   In  addition,  the underdrain prevents loss  of  the  media
with the  water, and during the backwash  cycle it provides  even
 flow distribution  over the bed.  Failure to dissipate  the  veloc-
 ity head  during the filter or backwash cycle  will  result in  bed
upset  and the need for major repairs.

 Several  standard  approaches  are  employed for filter underdrains.
The simplest one  consists of a parallel  porous  pipe imbedded
 under  a layer of  coarse gravel  and manifolded to a header pipe
 for effluent removal.   Other approaches  to  the underdrain system
 are known as the Leopold and Wheeler filter bottoms.   Both of
 these  incorporate  false concrete bottoms with specific porosity
 configurations to provide drainage and velocity head dissipation.

 Filter system operation may be manual or automatic.  The filter
 backwash cycle may be on a timed basis,  a pressure drop basis
 with a terminal value which triggers backwash,  or  a solids carry-
 over basis from turbidity monitoring of the outlet stream.  All
 of these schemes have been used sue cessfully.

 Application and Performance.  Wastewater treatment plants often
 use granular bed filters tor polishing after clarification, sedi-
 mentation, or other similar operations.  Granular  bed filtration
 thus has potential application to  nearly all industrial plants.
                                239

-------
 Chemical additives which enhance the upstream treatment eauinment
 may or may not be compatible with or enhance the filtration pro-
 cess.  Normal operation flow rates for various types of filters
 are as follows:
       Slow Sand
       Rapid Sand
       High Rate Mixed Media
 2.04 - 5.30 1/sq m-hr
40.74 - 51.48 1/sq m-hr
81.48 - 122.22 1/sq m-hr
 Suspended solids are commonly removed from wastewater streams by
 £f}£erifS through a deeP °-3 to 0.9 m (1 to 3 feet) granular
 tilter bed.   The porous bed formed by the granular media can be
 designed to remove practically all suspended particles.   Even
 colloidal suspensions (roughly 1 to 100 microns) are adsorbed on
 the surface of the media grains as they pass in close proximity
 in the narrow bed passages.

 Properly operated filters following some preliminary treatment to
 reduce suspended solids below 200 mg/1 should produce water with
 less  than 10 mg/1 TSS.   For example,  multimedia filters  produced
 the effluent qualities  shown in Table VII-9.

 Advantages and Limitations.   The principal advantages of granular
 bed filtration are its  comparatively  (to other filters)  low ini-
 tial  and operating costs,  reduced land requirements over othe>-
 methods  to achieve the  same  level of  solids  removal,  and elimina-
 tion  of chemical additions  to the discharge  stream.   However  the
 filter may require preliminary treatment if  the solids level'is
 high  Cover 100 mg/1).   Operator training must be somewhat exten-
 sive  due to  the controls  and periodic backwashing involved,  and
 backwash must be stored and  dewatered for economical  disposal.

 Operational  Factors.  Reliability:  The  recent improvements  in
 f7^er technol°gy  have  significantly  improved filtration relia-
 bility.   Control systems,  improved designs,  and good  operating
 procedures have made  filtration a highly reliable method of  water
 treatment.

Maintainability:   Deep  bed filters  may be operated with  either
manual or  automatic backwash.   In either case,  they must  be  peri-
odically inspected for  media attrition,  partial  plugging,  and
leakage.  Where backwashing  is  not used,  collected solids  must  be
removed  by shoveling, and filter media must be  at least  partially
replaced.                                                r        J
                                           )
Solid Waste Aspects:  Filter backwash is  generally recycled
within  the wastewater treatment  system,  so that  the solids ulti-
mately appear  in the clarifier  sludge stream  for  subsequent
dewatering.  Alternatively,  the  backwash stream  may be. dewatered
directly or, if there is no backwash,  the collected solids may be
                              240

-------
disposed of in a suitable landfill.  In either of these situa-
tions there is a solids disposal problem similar to that of
clarifiers.

Demonstration Status.  Deep bed filters are in common use in
municipal treatment plants.  Their use in polishing industrial
clarifier effluent is increasing, and the technology is proven
and conventional.  Granular bed filtration is currently used at
six copper forming plants.

Pressure Filtration

Pressure filtration works by pumping the liquid through a filter
material which is impenetrable to the solid phase.  The positive
pressure exerted by the feed pumps or other mechanical means pro-
vides the pressure differential which is the principal driving
force.

A typical pressure filtration unit consists of a number of plates
or trays which are held rigidly in a frame to ensure alignment
and which are pressed together between a fixed end and a travel-
ing end.  On the surface of each plate is mounted a filter made
of cloth or a synthetic fiber.  The feett stream is pumped into
the unit and passes through holes in the trays along the length
of the press until the cavities or chambers between the trays are
completely filled.  The solids are then entrapped, and a cake
begins to  form on the surface of the filter material.  The water
passes through the fibers, and the solids are retained.

At the bottom of the trays are drainage ports.  The filtrate is
collected  and discharged to a common drain.  As the filter medium
becomes coated with  sludge, the flow of filtrate through the
filter drops  sharply, indicating that the capacity of the filter
has been exhausted.  The unit must then be cleaned of the sludge.
After the  cleaning or replacement  of the filter media, the unit
is again ready for operation.

Application and Performance.  Pressure filtration may be used in
copper  forming for sludge  dewatering and also  for direct removal
of precipitated and  other  suspended solids from wastewater.

Because dewatering is such a common operation  in treatment sys-
tems, pressure filtration  is a  technique which can be  found  in
many  industries  concerned  with  removing solids from their waste
stream.
                                241

-------
 In a typical pressure filter, chemically preconditioned  sludge
 detained in the unit for one to three hours under pressures vary-
 ing from 5 to 13 atmospheres exhibited a final dry  solids  content
 between 25 and 50 percent.               i
                                          i
 Advantages and Limitations.  The pressures which may be  applied
 to a sludge for removal of water by filter presses  that  are
 currently available range from 5 to 13 atmospheres.  As  a  result
 pressure filtration may reduce the amount of chemical pretreat-
 ment required for sludge dewatering.  Sludge retained in the form
 of the filter cake has a higher percentage of solids than  that
 from a centrifuge or vacuum filter.  Thus,  it can be easily
 accommodated by materials handling systems.

 As a primary solids removal technique, pressure filtration
 requires less space than clarification and  is well suited to
 streams with high solids loadings.   The sludge produced may be
 disposed of without further dewatering.   The amount of sludge is
 increased by the use of filter precoat materials  (usually dia-
 tomaceous earth).   Also, cloth pressure filters often do not
 achieve as  high a degree of effluent clarification as clarifiers
 or granular media filters.                ,
                                          j
 Two disadvantages  associated with pressure  filtration in the past
 have been the short life of the filtjer cloths and lack of auto-
 mation.   New synthetic  fibers have  largely  offset the first of
 these problems.  Also,  units with automatic feeding and pressing
 cycles  are  now  available.                                       s
                                          |

 For larger  operations,  the  relatively  high  space  requirements,  as
 compared to those  of a  centrifuge,  could  be prohibitive in some
 situations.
                                          i

 Operational Factors.  Reliability:  With  proper -pretreatment,
 design,  and control,  pressure filtration  is  a highly dependable
 system.                                   :

Maintainability:  Maintenance consists of periodic  cleaning or
 replacement  of  the  filter media, drainage grids,  drainage piping,
 filter pans, and other parts  of the system.  If the  removal of
 the  sludge  cake is  not automated, additional  time  is  required  for
this operation.                           :

Solid Waste Aspects:  Because it is generally drier  than  other
types of sludges, the filter  sludge cake can be handled with
relative ease.  The accumulated sludge may be disposed by any of
the accepted procedures  depending on its chemical composition.
The levels of toxic metals present in sludge from treating
aluminum forming wastewater necessitate proper disposal.
                               242

-------
Demonstration Status.  Pressure filtration is a commonly used
technology in many commercial applications.  No copper forming
plants use pressure filtration for sludge dewatering.

Settling

Settling is a process which removes solid particles  from a liquid
matrix by gravitational force.  This is done by reducing the
velocity of the feed stream in a large volume tank or lagoon so
that gravitational settling can occur.  Figure VII-7 shows two
typical settling devices.

Settling is often preceded by chemical precipitation which
converts dissolved pollutants to solid form and by coagulation
which enhances settling by coagulating suspended precipitates
into larger, faster settling particles.

If no chemical pretreatment is used, the wastewater  is fed into  a
tank or lagoon where it loses velocity and the suspended solids
are allowed to settle out.  Long retention times are generally
required.  Accumulated sludge can be collected either periodi-
cally or continuously and either manually or mechanically.
Simple settling, however, may require excessively  large catch-
ments, and long retention times  (days as compared with hours) to
achieve high removal efficiencies.  Because of this, addition of
settling aids such as alum or polymeric flocculants  is often
economically attractive.

In practice, chemical precipitation often  precedes  settling, and
inorganic coagulants or polyelectrolytic flocculants are usually
added as well.  Common coagulants  include  sodium sulfate,  sodium
aluminate, ferrous or ferric  sulfate, and  ferric chloride.
Organic polyelectrolytes vary in structure, but all  usually  form
larger floe particles than coagulants used alone.

Following this pretreatment,  the wastewater can be  fed into  a
holding tank or  lagoon for settling, but is more often piped  into
a clarifier for the  same purpose.  A clarifier reduces space
requirements, reduces retention  time,  and  increases  solids
removal efficiency.  Conventional  clarifiers  generally consist  of
a circular  or rectangular  tank with  a. mechanical sludge  collect-
ing  device or with a sloping  funnel-shaped bottom  designed  for
sludge collection.   In advanced  settling devices,  inclined
plates, slanted  tubes, or  a  lamellar network  may be  included
within the  clarifier tank  in order to  increase  the effective
settling  area,  increasing  capacity.  A fraction of the  sludge
stream is  often recirculated to  the  inlet,  promoting formation  of
a denser  sludge.
                                243

-------
 Application and Performance.  Settling and clarification are used
 in the copper forming category to remove precipitated metals.
 Settling can be used to remove most suspended solids in a partic-
 ular waste stream;  thus it is used extensively by many different
 industrial waste treatment facilities.  Because most metal ion
 pollutants are readily converted to solid metal hydroxide precip-
 itates,  settling is of particular use in those industries associ-
 ated with metal production, metal finishing,  metal working,  and
 any other industry  with high concentrations of metal ions in
 their wastewaters.   In addition to toxic medals,  suitably pre-
 cipitated materials effectively removed by settling include
 aluminum,  iron, manganese, cobalt, antimony,  beryllium,
 molybdenum,  fluoride,  phosphate, and many others.

 A properly^operated settling system can efficiently remove sus-
 pended solids,  precipitated metal hydroxides,  and other  impuri-
 ties from wastewater.   The performance of the process depends on
 a variety of factors,  including the density and particle size of
 the solids,  the effective charge on the suspended particles,  and
 the types  of chemicals  used in pretreatment.   The site of floccu-
 lant or  coagulant addition also may significantly influence  the
 effectiveness of clarification.   If the flocculant is subjected
 to too much  mixing  before entering the clarifier,  the complexes
 may be sheared  and  the  settling effectiveness  diminished.  At the
 same time,  the  flocculant must have sufficient mixing and reac-
 tion time  in order  for  effective set-up and settling to  occur.
 Plant personel  have observed that the line pr  trough leading  into
 the clarifier is often  the most efficient site for flocculant
 addition.  The  performance of simple settling  is  a function of
 the retention time,  particle size and density,  and the surface
 area of  the  basin.

 The data displayed  in Table VII-10 indicate1suspended solids
 removal  efficiencies in settling systems.

 The mean effluent TSS concentration obtained by the  plants shown
 in Table VII-10  is  10.1  mg/1.   Influent concentrations averaged
 838 mg/1.  The  maximum  effluent  TSS value reported is 2,3 mg/1.
 These plants  all use alkaline pH adjustment to precipitate metal
 hydroxides, and  most add a coagulant  or flocculant prior to
 settling.
                                            |

Advantages and Limitations.   The major advantage of  simple set-
 tling  is its  simplicity  as  demonstrated by the gravitational
 settling of solid particular  waste in a holding tank  or  lagoon.
The major problem with simple  settling  is the  long retention  time
necessary to  achieve an  acceptable effluent, especially  if the
 specific gravity of the  suspended  matter  is close  to that of
water.   Some  materials  cannot  be  effectively removed by simple
 settling alone.
                               244

-------
Settling performed in a clarifier is effective in removing slow-.
settling suspended matter in a shorter time and in less space
than a simple settling system.  Also, effluent quality is often
better from a clarifier.  The cost of installing and maintaining
a clarifier; however, is substantially greater than the costs
associated with simple settling.

Inclined plate, slant tube, and lamellar settlers have even
higher removal efficiencies than conventional clarifiers., and
greater capacities per unit area are possible.  Installed costs
for these advanced clarification systems are^claimed to be one
half the cost of conventional systems of similar capacity.

Operational Factors.  Reliability:  Settling can be a highly
reliable technology  for removing suspended  solids.  Sufficient
retention time and regular  sludge removal are important factors
affecting the reliability  of  all settling systems.  Proper con-
trol of pH  adjustment,  chemical precipitation, and coagulant or
flocculant  addition  are additional  factors  affecting settling
efficiencies in systems  (frequently clarifiers) where  these
methods are used.

Those  advanced  settlers using slanted  tubes,  inclined  plates,  or
a  lamellar  network may  require  prescreening of the waste  in  order
to eliminate any  fibrous materials  which could potentially  clog
the  system.  Some installations are especially vulnerable to
shock  loadings, as by storm water  runoff, but proper  system
design will prevent  this.

Maintainability:  When  clarifiers  or other  advanced  settling
devices  are used,  the associated  system utilized for  chemical
pretreatment and  sludge dragout must be maintained  on  a regular
basis. Routine maintenance of mechanical parts  is  also neces-
 sary.  Lagoons  require  little maintenance other  than  periodic
 sludge removal.

Demonstration  Status

 Settling represents the typical method of solids removal and is
 employed extensively in industrial waste treatment.   The advanced
 clarifiers are just beginning to appear in significant numbers in
 commercial applications.   Thirty-six copper forming plants  use
 sedimentation or clarification.

 Skimming

 Pollutants with a specific gravity less than water will often
 float unassisted to the surface of the wastewater.   Skimming  ^
 removes these floating wastes.  Skimming normally takes place in
 a tank designed to  allow the floating material to rise and remain
                                245

-------
                                            I
 on the surface, while the liquid flows to an outlet located below
 the floating layer.  Skimming devices are therefore suited to the
 removal of non-emulsified oils from raw waste streams.  Common
 skxmming mechanisms include the rotating drum type, which picks
 up oil from the surface of the water as it rotates.  A doctor
 blade scrapes oil from the drum and collects it in a trough for
 disposal or reuse.  The water portion is allowed to flow under
 the rotating drum.  Occasionally, an underflow baffle is
 installed after the drum;  this has the advantage of retaining any
 floating oil which escapes the drum skimmer.   The belt type
 skimmer is pulled vertically through the water, collecting oil
 which is scraped off from the surface and collected in a drum.
 Gravity separators (Figure VII-8),  such as the API type, utilize
 overflow and underflow baffles to skim a floating oil layer from
 the surface of the wastewater.  An overflow-underflow baffle
 allows a small amount of wastewater (the oil portion) to flow
 over into a trough for disposition or reuse while the majority of
 the water flows underneath the baffle.   This  is followed by an
 ?V^flow baffle> which is  set at a height relative to the first
 baffle such that only the  oil bearing portion will flow over the
 first baffle during normal plant operation.   A diffusion device
 such as  a vertical slot  baffle,  aids  in creating a uniform flow'
 through the system and increasing oil removal efficiency.

 Application and Performance.   Skimming  is applicable  to any waste
 stream containing pollutants  which  float  to  the surface.   It is
 commonly  used to remove  free  oil, grease,  and soaps.   Skimming is
 often used in conjunction  with air  flotation  or clarification in
 order to  increase its effectiveness.

 The removal efficiency of  a skimmer is  partly a function of the
 retention  time  of the water in the  tank.  Larger,  more  buoyant
 particles  require less retention  time than  smaller particles.
 Thus,  the  efficiency  also  depends on  the  composition  of the waste
 stream.  The  retention time required  to allow phase separation
 and subsequent  skimming  varies  from 1 to  15 minutes, depending on
 the wastewater  characteristics.

API or other  gravity-type  separators  tend to  be  more  suitable  for
use where the amount  of  surface oil flowing through the  system is
 continuous  and  substantial.  Drum and belt type  skimmers are
 applicable  to waste streams which evidence smaller  amounts  of
 floating oil  and where surges  of floating oil are  not a  problem.
Using  an API separator system in conjunction with a drum type
 skimmer would be a very  effective method of removing floating
contaminants from non-emulsified oily waste streams.  Sampling
data shown  in Table VII-11 illustrate the capabilities of the
technology with both extremely high and moderate oil influent
levels.
                               246

-------
This data is intended to be illustrative of the very high level
of oil and grease removals attainable in a simple two stage^oil
removal system.  Based on the performance of installations in a
variety of manufacturing plants and permit requirements that are
constantly achieved, it is determined that effluent oil levels
may be reliably reduced below 10 mg/1 with moderate influent
concentrations.  Very high concentrations of oil such as the 22
percent shown in Table VII-11 may require two step treatment to
achieve this level.

Skimming which removes oil may also be used to remove base levels
of organics.  Plant sampling data show that many organic com-
pounds tend to be removed in standard wastewater treatment equip-
ment.  Oil separation not only removes oil but also organics that
are more soluble in oil than in water.  Clarification removes
organic solids directly and probably removes dissolved organics
by adsorption on inorganic solids.

The source of these organic pollutants is not always known with
certainty, although in metal forming operations they seem to
derive mainly from various process lubricants.  They are also
sometimes present in the plant water supply, as additives to
proprietary formulations of cleaners* or due to leaching from
plastic liners and other materials.

High molecular weight organics in particular are much more solu-
ble in organic solvents than in water.  Thus they are much more
concentrated in the oil phase that is skimmed than in the waste-
water.  The ratio of solubilities of a compound in oil and water
phases is called the partition coefficient.  The logarithm of the
partition coefficients  for 15 polynuclear aromatic hydrocarbon
 (PAH) compounds in octanol and water are:
          PAH Priority  Pollutant

         1.   Acenaphthene
        30.   Fluoranthene
        72.   Benzo(a)anthracene
        73.   Benzo(a)pyrene
        74.   3,4-Benzofluoranthene
        75.   Benzo(k)fluoranthene
        76.   Chrysene
        77.   Acenaphthylene
        78.   A.nthracene
        79.   Benzo(ghi)perylene
        80.   Fluorene
        81.   Phenanthrene
        82.   Dibenzo(a,h)anthracene
        83.   Indeno(l,2,3,cd)pyrene
        84.   Pyrene
  Log Octanol/Water
Partition Coefficient

        4.33
        5.33
        5.61
        6.04
        6.57
        6.84
        5.61
        4.07
        4.45
        7.23
        4.18
        4.46
          .97
          .66
5,
7
5.32
                                247

-------
 Plant sampling data show that many organic:compounds tend to be
 removed in standard wastewater treatment equipment.   Oil separa-
 tion not only removes oil but also organics  that are more soluble
 in oil than in water.  Clarification removes organic solids
 directly and probably removes dissolved organics by  adsorption on
 inorganic solids.
                                           |
 Figure VII-9 shows  the relationship between  the concentrations of
 total toxic organics and oil and grease in wastewater samples
 from copper forming plants.   It can be seen  that if  a daily
 maximum oil and grease concentration of 20 mg/1 is achieved,  the
 concentration of total toxic organics is expected to be  below 0.5
 mg/1.   This conclusion is also supported by  data from copper
 forming plants which practice oil skimming on wastewaters  which
 contain toxic organics as well as oil and grease.  Data  from
 three days  of sampling at two copper forming plants  which  prac-
 tice oil skimming and achieve effluent oil and grease concentra-
 tions  of 20 mg/1 or less are presented in Table VII-12.  It can
 be seen that the concentration of total toxic organics in  these
 effluent samples never exceeds 0.31 mg/1.
                                           I
 The  unit operation  most applicable to removal of trace toxic
 organics is adsorption,  and  chemical oxidation is another  possi-
 bility.   Biological degradation is not generally applicable
 because the organics  are not present in sufficient concentration
 to sustain  a biomass  and because most of the organics are
 resistant to biodegradation.

 Advantages  and Limitations.   Skimming as a pretreatment  is  effec-
 tive in removing naturally floating waste  material.   It  also
 improves the performance of  subsequent downstream treatments.

Many pollutants, particularly dispersed or emulsified oil,  will
 not  float "naturally"  but require  additional treatments.  There-
 fore,  skimming alone  may not  remove all the  pollutants capable  of
being removed  by air  flotation or  other more sophisticated  tech-
 nologies .

Operational  Factors.  Reliability:   Because  of  its simplicity,
 skimming  is  a  very  reliable  technique.

Maintainability:  The  skimming  mechanism requires periodic
 lubrication,  adjustment,  and  replacement of  worn parts.

Solid Waste Aspects:  The collected layer  of debris  must be
 disposed of by contractor removal,  landfill,   or incineration.
Because  relatively  large  quantities  of  water are present in the
collected wastes, incineration  is not always  a viable disposal
method.                                    !
Demonstration Status.  Skimming is a common operation utilized
extensively by industrial waste treatment systems.  It is
presently used at 10 copper forming plants.j
                               248

-------
Chemical Emulsion Breaking

Chemical treatment is often used to break stable  oil-in-water
(0-W) emulsions.  An 0-W emuls'ion consists of oil dispersed in
water, stabilized by electrical charges and  emulsifying  agents.
A stable emulsion will not separate or break down without  some
form of treatment.

Once an emulsion is broken, the difference in specific gravities
allows the oil  to float to the surface of the water.  Solids^usu-
ally form a layer between the oil and water, since  some  oil  is
retained ,in the solids.  The longer the retention time,  the more
complete and  distinct the separation between the  oil, solids,  and
water will be.  Often other methods of gravity  differential
separation, such as air flotation or rotational separation (e.g.,
centrifugation), are used to enhance and speed  separation.  ^A
schematic flow  diagram of one type  of application is  shown in
Figure VII-10.

The major equipment required for  chemical emulsion  breaking
includes:  reaction chambers with agitators, chemical storage
tanks, chemical feed  systems, pumps, and piping.

Emulsifiers may be used in the plant: to aid  in  stabilizing or
forming  emulsions.  Emulsifiers  are surface-active  agents which
alter the characteristics of the  oil and water  interface.   These
sufactants have rather  long polar molecules. One end of the
molec-ale  is particularly  soluble  in water  (e.g.,  carboxyl, sul-
fate, hydroxyl, or  sulfonate groups) and  the other end is readily
soluble  in oils (an organic  group which  varies  greatly with the
different  surfactant  type).  Thus,  the  surfactant emulsifies or
suspends  the  organic  material  (oil) in water.   Emulsifiers also
lower the surface  tension of  the 0-W emulsion as a result of
solvation and ionic  complexing.   These  emulsions must be
destabilized  in the  treatment  system.

Application  and Performance.   Emulsion breaking is applicable to
waste streams containing  emulsified oils  or lubricants such as
 rolling and  drawing emulsions.

Treatment of spent 0-W emulsions involves the use of chemicals to
break the emulsion followed by gravity differential separation.
 Factors to be  considered for breaking emulsions are type of chem-
 icals,  dosage  and sequence of addition,  pH, mechanical shear and
 agitation,  heat,  and retention time.

 Chemicals,  e.g.,  polymers,  alum, ferric chloride, and organic
 emulsion breakers, break emulsions by neutralizing repulsive
 charges between particles,  precipitating or salting out emul-
 sifying agents, or altering the interfacial film between the
                                249

-------
 oil and water so it is readily broken.  Reactive cations, e.g.,
 H(+l), Al(+3), Fe(+3), and cationic polymers, are particularly
 effective in breaking dilute 0-W emulsions.  Once the charges
 have been neutralized or the ihterfacial film broken, the small
 oil droplets and suspended solids wil be adsorbed on the surface
 of the floe that is formed, or break out and float to the top.
 Various types of emulsion-breaking chemicals are used for the
 various types of oils.

 If more than one chemical is required, the sequence of addition
 can make quite a difference in both breaking efficiency and
 chemical dosages.
                                            i
 pH plays an important role in emulsion breaking, especially if
 cationic inorganic chemicals, such as alum,; are used as coagu-
 lants.  A depressed pH in the range of 2 to 4 keeps the aluminum
 ion in its most positive state where it can function most effec-
 tively for charge  neutralization.   After some of the oil is
 broken free and skimmed,  raising the pH into the 6 to 8 range
 with lime or caustic will cause the aluminum to hydrolyze and
 precipitate as aluminum hydroxide.   This floe entraps or adsorbs
 destabilized oil droplets which can then be separated from the
 water phase.   Cationic polymers can break emulsions over a wider
 pH range and thus  avoid acid corrosion and the additional sludge
 generated from neutralization;  however,  an inorganic flocculant
 is usually required to supplement  the polymer emulsion breaker's
 adsorptive properties.

 Mixing is important in breaking 0-W emulsions.   Proper chemical
 feed and dispersion is  required for effective results.   Mixing
 also causes collisions  which help  break  the emulsion,  and sub-
 sequently helps  to  agglomerate  droplets.

 In all emulsions, the  mix of two immiscible liquids  has  a spe-
 cific gravity very  close  to that of water.   Heating lowers  the
 viscosity and increases the apparent specific gravity differen-
 tial between oil and water.   Heating also increases  the  frequency
 of droplet collisions, which helps  to rupture the  interfacial
 film.
                                            j
 Oil  and grease and  suspended solids  performance data are shown in
 Table VII-13.  Data were  obtained  from sampling at  operating
 plants and a  review of  the current  literature.   This  type of
 treatment  is  proven to be reliable  and is  considered  the current
 state-of-the-art for copper forming emulsified  oily  wastewaters.

Advantages  and Limitations.   Advantages  gained  from  the  use of
 chemicals  for  breaking 0-W emulsions  are  the  high removal effi-
 ciency potential and the  possibility of  reclaiming the oily
waste.  Disadvantages are  corrosion  problems  associated  with
                               250

-------
acid-alum systems, skilled operator requirements for batch treat-
ment, chemical sludges produced, and poor cost-effectiveness for
low oil concentrations.

Operational Factors.  Reliability:  Chemical emulsion breaking is
a very reliable process.  The main control parameters, pH and
temperature, are fairly easy to control.

Maintainability:  Maintenance is required on pumps, motors, and
valves, as well as periodic cleaning of the treatment tank to
remove any accumulated solids.  Energy use is limited to mixers
and pump s.

Solid Waste Aspects:  The surface oil and oily sludge produced
are usually hauled away by a licensed contractor.  If the recov-
ered oil has a sufficiently low percentage of water, it may be
burned for its fuel value or processed and reused.

Demonstration Status.  Sixteen plants in the aluminum forming
category currently break emulsions with chemicals.  Eight plants
chemically break  spent rolling oil emulsions with  chemicals, one
plant breaks its rolling and drawing emulsions, one plant breaks
its  rolling oils  and  degreasing solvent, one plant breaks its
direct chill casting  contact cooling water, scrubber liquor, and
sawing oil, and one plant breaks  its direct chill  casting contact
cooling water and extrusion press heat treatment contact cooling
water.  No plants in  the copper forming industry currently use
chemical emulsion breaking.

Thermal Emulsion  Breaking

Dispersed oil droplets in a spent  emulsion can be  destabilized by
the  application of  heat to the waste.  One type  of technology
commonly used, in  the  metals and mechanical products industries is
the  evaporation-decantation-condensation process,  also  called
thermal emulsion  breaking  (TEB),  which separates the  emulsion
waste into  distilled  water, oils  and  other  floating materials,
and  sludge.  Raw  waste is  fed to  a main reaction chamber.  Warm
air  is passed over  a  large revolving  drum which  is partially  sub-
merged in the waste.   Some water  evaporates  from the  surface  of
the  drum  and  is carried upward  through  a  filter  and a condensing
unit.  The  condensed  water is discharged or reused as process
makeup, while the air is  reheated and returned  to  the evaporation
stage.  As  the water  evaporates in the  main  chamber,  oil  concen-
tration  increases.  This  enhances agglomeration  and gravity  sepa-
ration of oils.   The  separated  oils and other  floating  materials
 flow over a weir  into a decanting chamber.  A  rotating  drum
skimmer picks up  oil  from the surface of  the decanting  chamber
 and  discharges  it for possible  reprocessing  or contractor
removal.  Meanwhile,  oily water is being  drawn from the bottom of
                                251

-------
 the decanting chamber, reheated, and sent back into the main con-
 veyorized chamber.   Solids which settle out in the main chamber
 are removed by a conveyor belt.  This conveyor belt, called a
 flight scraper, moves slowly so as not to interfere with the
 settling of suspended solids.

 Application and Performance.  Thermal emulsion breaking technol-
 ogy can be applied  to the treatment of spent emulsions in the
 copper forming category.

 The performance of  a thermal emulsion breaker is dependent
 primarily on the characteristics of the raw waste and proper
 maintenance and functioning of the process components.  Some
 emulsions may contain volatile compounds which could escape with
 the distilled water.   In  systems where the water is recycled back
 to  process; however,  this problem is essentially elminated.
 Experience in at least two copper forming plants has shown that
 trace  organics or other contaminants found (in the condensed water
 will not adversely  affect the lubricants when this water is used
 for process emulsions.  In one copper forming plant, typical oil
 and grease level in the condensed water was 1 mg/1.
                                            ]
 Advantages and Limitations.   Advantages of the thermal emulsion
 breaking process include  high percentages of oil removal (at
 least  99 percent in most  cases),  the separation of floating oil
 from settleable sludge  solids,  and the production of distilled
 water  which is available  for process reuse.   In addition,  no
 chemicals  are required  and the operation is automated,  factors
 which  reduce operating costs.   Disadvantages of the process are
 the  energy requirement  for water  evaporation and,  if intermit-
 tently operated,  the  necessary installation of a large storage
 tank.

 Operational Factors.  Reliability:   Thermal  emulsion breaking is
 a very reliable process for  the treatment of emulsified oil
wastes.

Maintainability:  The thermal  emulsion breaking process requires
 minimal  routine maintenance  of the process  components,  and peri-
 odic disposal  of the  sludge  and oil.
                                            i
 Solid Waste Aspects:  The  thermal  emulsion breaking process
 generates  sludge  which must  be  properly disposed of.

Demonstration  Status.  Thermal  emulsion breaking is  used in
metals and mechanical products  industries.  ;It  is  a  proven method
of effectively treating emulsified wastes.   Six copper  forming
plants currently  use thermal emulsion  breaking.
                               252

-------
MAJOR TECHNOLOGY EFFECTIVENESS

The performance of individual treatment technologies was pre-
sented above.  Performance of operating systems is discussed
here.  Two different systems are considerred:  LSeS (hydroxide
precipitation and sedimentation or lime and settle) and LSScF
(hydroxide precipitation, sedimentation, and  filtration or  lime,
settle, and filter).  Subsequently, an analysis of effectiveness
of such systems is made to develop one-day maximum and ten-day
and thirty-day average concentration levels to be used in regu-
lating pollutants.  Evaluation of the L&S and the LS&F systems  is
carried out on the assumption that chemical reduction of chro-
mium, cyanide precipitation, oil skimming, and emulsion breaking
are installed and operating properly where appropriate.

LS»S Performance - Combined Metals Data Base

Before proposal, chemical analysis data were  collected of raw
waste  (treatment influent) and treated waste  (treatment effluent)
from 55 plants (126 data days) sampled by EPA (or its contractor)
using EPA  sampling and chemical  analysis protocols.  These  data
are the data base for determining the effectiveness of L&S  tech-
nology.  Each of these plants belongs to at  least one of the
following  industry categories:   aluminum forming, battery
manufacturing, coil coating, copper  forming,  electroplating and
porcelain  enameling.  All of the plants employ pH adjustment and
hydroxide  precipitation using  lime or caustic, followed by
settling  (tank, lagoon or clarifier) for solids removal.  Most
also  add  a coagulant  or  flocculant prior to  solids removal.

An  analysis  of this data was presented  in  the development  docu-
ments  for  the proposed regulations for  coil  coating and porcelain
enameling  (January 1981).  In  response  to  the proposal,  some
commenters claimed that  it was  inappropriate  to use data  from
some  categories  for regulation of  other categories.   In response
to  these  comments, the Agency  reanalyzed the  data.  An analysis
of  variance was  applied  to the data  for the  126  days  of  sampling
to  test  the hypothesis of homogeneous plant  mean  raw  and  treated
effluent  levels  across  categories  by pollutant.   This  analysis  is
described  in the report,  "A  Statistical Analysis  of the Combined
Metals Industries Effluent Data" which  is  in the administrative
record supporting this rulemaking.   The main conclusion  drawn
 from the analysis of  variance  is that,  with  the  exception of
electroplating,  the  categories are generally homogeneous  with
regard to mean pollutant concentrations in both raw  and  treated
 effluent.   That  is, when data  from electroplating facilities are
 included in the analysis,  the  hypothesis  of  homogeneity  across
 categories is rejected.   When  the  electroplating data are removed
 from the analysis  the conclusion changes  substantially and the
hypothesis of homogeneity across categories  is not  rejected.   On
                                253

-------
 the basis  of this  analysis,  the electroplating data were removed
 from the data base used to determine limitations.   Cases that
 appeared to  be marginally different were not unexpected (such as
 copper  in  copper forming and lead in lead battery  manufacturing)
 and were accommodated in developing limitations by using the
 larger  values obtained from the marginally different category to
 characterize the entire data set.

 The statistical analysis provides support for the  technical engi-
 neering judgement  that electroplating wastewaters  are different
 from most  metal processing wastewater.   These differences  may be
 further explained  by  differences  in the  constituents and relative
 amounts of pollutants in the raw  wastewaters.   Therefore,  the
 wastewater data derived from plants that only electroplate are
 not used in  developing limitations  for the aluminum forming
 category.
                                           i

 After removing the electroplating data,  data from  21 plants and
 52  days of sampling remained.

 For the purpose of developing treatment  effectiveness,  certain
 additional data were  deleted from the data base before  examina-
 tion for homogeneity.   These deletions were made to ensure that
 the data reflect properly  operated  treatment systems and actual
 pollutant  removal.  The following criteria were used in making
 these deletions:

        Plants  where  malfunctioning processes  or treatment
        systems at time of sampling were identified.

     -  Data days  where pH was  less than 7.0 or TSS was  greater
        than 50 mg/1.   (This  is a prima^facie  indication of poor
        operation.)

        Data points where  the raw value  was  too low to  assure
        actual  pollutant removal  occurred (i.e., less than 0.1
        mg/1 of pollutant  in raw waste).

Collectively,  these selection criteria ensure  that  the  data are
 from properly  operating lime  and  settle  treatment  facilities.
The remaining  data are  displayed  graphically in Figures  VII-11  to
VII-19.  This  common  or combined metals  data base provides  a more
 sound and  usable basis  for estimating treatment effectiveness and
statistical  variability of lime and settle technology than  the
available  data  from any one  category.

One-Day Effluent Values

The basic  assumption  underlying the determination of  treatment
effectiveness is that the  data  for  a  particular pollutant  are
                               254

-------
lognormally distributed by plant.  The lognormal has been found
to provide a satisfactory fit to plant effluent data in a number
of effluent guidelines categories.  In, the case of the combined
metal categories data base, there are too few data from any one
plant to verify formally the lognormal assumption. ^ Thus, we
assumed measurements of each pollutant from a particular plant,
denoted by X, follow a lognormal distribution with a log mean u
and log variance 02.  The mean, variance, and 99th percentile
of X are then:

     mean of X - E(X) - exp ( U+ a2/?.)

     variance of X = V(X) - exp(2 u+a2)  [exp(a2) - 1]
    99th percentile
                            = exp( U+ 2.33a)
where exp is e, the base of  the natural  logarithm.  The  term
lognormal is used because the logarithm  of X has  a normal  dis-
tribution with mean u and variances2.   Using  the basic
assumption of log normality  the actual treatment  effectiveness
was determined using a  lognormal  distribution  that, in a sense,
approximates the distribution of  an  average of the plants  in the
data base, i.e., an "average plant"  distribution. The notion of
an "average plant" distribution is not a strict statistical  con-
cept but is used here to determine  limits that would  represent
the performance capability of an  average of the plants in the
data base.

This "average plant" distribution for a  particular pollutant was
developed as  follows:   the log mean  was  determined by taking the
average  of all  the observations  for  the  pollutant across plants.
The log  variance was determined by  the pooled  within  plant
variance.  This  is the  weighted  average  of the plant  variances.
Thus, the log mean represents  the average of  all the  data for the
pollutant and the  log variance  represents the  average of the
plant log variances or  average plant variability for  the
pollutant.

The  one-day  effluent values  were determined as follows:

Let Xj_j  - the jth observation on a particular pollutant at
plant  3.  where
                        X
           I
          Ji
Then

where
               1 ,
              total number of plants
              number of observations at plant i.
               In
          £J

          In means the natural logarithm.
                                255

-------
 Then
 where
           y = log mean over all plants

                I     Ji
             =  2     Z
                i=l   J-l

           n — total  number of observations

                I                          :
             -  S     Ji
and
        V(y)
pooled log variance


      (Ji-DSi*
                2
                     (Ji-1)
where
            — log variance at plant  i

               ii
               j-i   yx:i
           s log mean at plant i.         >

Thus, y and V(y) are the log mean and log variance, respectively,
of the lognormal distribution used to determine the treatment
effectiveness.  The estimated mean and 99th percentile of this
distribution form the basis for the  long term average and daily
maximum effluent limitations, respectively.  The estimates are
      mean
                   = exp(y)i|in(0.5V(y))

      99th percentile = X.99 = exp[y + 2.3;3Vv(y)]
where *K.) is a Bessel function and exp is e, the base of the
natural logarithms  (see Aitchison, J. and J. A. C. Brown, The
Lognormal Distribution, Cambridge University Press, 1963).  In
cases where zeros were present in the data,, a generalized form of
the lognormal, known as the delta distribution was used  (see
Aitchison and Brown, op. cit., Chapter 9).
                                          (
For certain pollutants, this  approach was modified slightly to
accommodate situations in which a category or categories stood
out as being marginally different from the others.  For  instance,
after excluding the electroplating data and other data that did
                               256

-------
not reflect pollutant removal or proper treatment, the effluent
copper data from the copper forming plants were statistically
significantly greater than the copper data from the other plants.
Thus, copper effluent values shown in Table VII-14 are based only
on the copper effluent data from the copper forming plants.  That
is, the log mean for copper is the mean of the logs of all copper
values from the copper forming plants only and the log variance
is the pooled log variance of the copper forming plant data only.
In the case of cadmium, after excluding the electroplating data
and data that did not reflect removal or proper treatment, there
were insufficient data to estimate the log variance for cadmium.
The variance used to determine the values shown in Table VII-14
for cadmium was estimated by pooling the within plant variances
for all the other metals.  Thus, the cadmium variability is the
average of the plant variability averaged over all the other
metals.  The log mean for cadmium is the mean of the logs of the
cadmium observations only.  A complete discussion of the data  and
calculations for all the metals is contained in the administra-
tive record for this rulemaking.

Average Effluent Values

Average effluent values that form the basis for the monthly
limitations were developed in a manner consistent with the method
used to develop one-day treatment effectiveness in that the log-
normal distribution used for the one-day effluent values was also
used as the basis for the average values.  That is, we assume  a
number of consecutive measurements are drawn from the distribu-
tion of daily measurements.  The approach used for the 10 mea-
surements valxies was employed previously for the electroplating
category  (see "Development Document  for Existing Sources
Pretreatment Standards for the Electroplating Point Source
Category," EPA 440/1-79/003, U.S. Environmental Protection  .
Agency, Washington, D.C., August, 1979).  That is, the distri-
bution of the average of 10 samples  from a lognormal was
approximated by another lognormal distribution.  Although the
approximation is not precise theoretically, there  is empirical
evidence based on effluent data from a number of categories that
the  lognormal is an adequate approximation for the distribution
of small samples.  In the course of  previous work  the approxi-
mation was verified in a computer simulation study.  The  average
values were developed assuming independence of the observations
although  no particular sampling scheme was assumed.

Ten-Sample Average:

The  formulas  for the 10-sample  limitations were derived  on  the
basis  of  simple relationships between  the mean and variance of
the  distributions of the daily pollutant measurements and  the
average of 10 measurements.  We assume the daily  concentration
                               257

-------
 measurements  for a particular pollutant,  denoted by X,  follow  a
 lognormal  distribution with log  mean  and  log  variance denoted  by
 P and a^   respectively.   Let XIQ denote the mean of 10
 consecutive measurements.   The following  relationships  then hold
 assuming the  daily measurements  are independent:
     mean of
                           =  E(X)
     variance  of XIQ - V(XIQ)  - V(X)  *  10.

Where E(X) and V(X) are  the  mean  and_variance  of X, respectively,
defined above.  We then  assume that X^Q  follows a lognormal
distribution with log meanuio and log  standard deviation
  10
          mean and variance of
                                   are  then
            - exp(y1() + 0.5a210)

     V(X10) - exp(2v10 +
Now,
         and
                  can ^e derived in terms of  u and a2 as
                    + o.51n[l

                   (exp(a2) -
                                 (exp(a2 -
Therefore, U IQ and cr2^Q can be estimated using the above
relationships and the estimates of U and a;2 obtained for the
underlying lognormal distribution.  The 10 sample limitation
value was determined by the estimate of the approximate 99th
percentile of the distribution of the 10 sample average given by

              = exp(uio + 2.33 a10)
              A
              OIQ are the estimates of UIQ and
where UIQ
respectively.

30 Sample Average:
                                          i

The average values based on 30 measurements are determined on the
basis of a statistical result known as the Central Limit Theorem.
This Theorem states that, under general and nonrestrictive
assumptions, the distribution of a sum of a number of random
variables, say n, is approximated by the normal distribution.
The approximation improves as the number of variables, n,
increases.  The Theorem is quite general in that no particular
distributional form is assumed for the distribution of the
individual variables.  In most applications (as in approximating
the distribution of 30-day averages) the Theorem is used to
approximate the distribution of the average of n observations of
a random variable.  The result makes it possible to compute
                               258

-------
approximate probability statements about the average in a wide
range of cases.  For instance, it is possible to compute a value
below which a specified percentage Ae.g., 99 percent) of the
averlgls of n observations are likely to fall.  Most textbooks
state that 25 or 30 observations are sufficient for tne
approximation to be valid.  In applying the Theorem to the    _
determination of 30 day average effluent values, we approximate
the distribution of the average of 30 observations _ drawn from the
distribution of daily measurements and use the estimated yytn
percentile of this distribution.  The monthly limitations based
on 10 consecutive measurements were determined using the log-
normal approximation described above because 10 measurements
were, in this  case, considered too small a number  for use of  the
Central Limit Theorem.

30 Sample Average Calculation

The  formulas for the 30 sample average were based  on an  applica-
tion of  the Central Limit Theorem.  According to  the Theorem  the
average  of 30  observations drawn  from the  distribution of daily
measurements,  denoted  by  X30, is  approximately  normally  dis-
tributed.  The mean and variance  of X3o  are

      mean  of X30 - E(X30) = E(X)

      variance  of X3Q = V(X3o) - V(X) *  30 .

The 30  sample  average  value was  determined by the estimate  of the
 approximate 99th percentile of the distribution of the 30  sample
 average given  by
A
         A
                                   _

      X30(.99) = E(X) + 2.33-V VA(X) * 30

 where     EA(X) = exp(y)ifn(0.5V(y) )

 and       VA(X) = exp(2y)!>n(2V(y)) - i|m { (5Z2.)


 The formulas  for EA(X) and V^X) are estimates of E(X) and_V(X) ,
 respectively  given  in Aitchison, J .. and J. A. C. Brown  The
 T.ngLrmal Distribution, Cambridge University Press, 1963, page
 45?

 Application

 In response  to the  proposed coil coating and porcelain  enameling
 regulations,  the Agency received comments  pointing out  that  per
 mils usually required  less than  30 samples to be taken  during a
 mon?h  while> theqmonthly average  used  as  the basis  for permits and
 pretreatment requirements  is  based on the  average  of 30 samples.
                                259

-------
  In applying the treatment effectiveness values to regulations we
  have  considered the comments,  examined the sampling frequency
  SS™*    57 ^ Permits>  and  considered the changl in valuSs of
  averages  depending  on the number of consecutive slmpling days in
  the averages.   The  most common frequency of sampling requiSd in
  permits is  about 10 samples  per month or slightly greater than
                     99th. P^cent iles of the dStSbSttSn of
                            samPlin§ days are not  substantially
                          Percentile  of the distribution's 30  day
  «™n     mPare^ *>  ^e one-day  maximum,  the 10-day average is
  about 80  percent of the difference  between one and 30-day   §
  for r^nt.??nCe>  the 10"1a?  averaSe Provides a reasonable^ basis
             1                          °f
 The monthly average is to be achieved in all permits and pre-
 treatment standards regardless of the number of  samples required
 authority!7        averaged by the -permit or the pretreatment


 Additional Pollutants
          °f other Pol:l-utant parameters were considered with
        to the performance of lime and settle treatment systems in
          thS? fr°? industrial wastewater.  Performance Sta for
 the      am*   ^1S n0t reSdily availablea so data available to
 the Agency in other categories has been selectively used to
 determine the long-term average performance of lime and settle
 technology for each pollutant.  These data indicatJ Sat the
 concentrations shown in Table VII-15 are reliably attaiSablS with
 hydroxide precipitation and settling.  The precipitation of
 silver appears to be accomplished by alkaline chloride precipi-
 tation and adequate chloride ions must be available for this
 reaction to occur.

 In  establishing which data were suitable for use in Table VII-15

 wI?er^aS5Sr2?r?h^eaVily w^f^:   ^ th* *ature of 'the waste-
 water,  and (2)  the  range of pollutants or ; pollutant matrix in  the
 raw wastewater.   These data have been selected from process^
 ™o g??er5te  ^solved metals  in the wastewater and which are
 IvafuaS £e?   °m- comPiexin§ a§ents.  The pollutant  matrix was
 evaluated by comparing the concentrations  of pollutants  found  in
 the raw wast ewaters  with the range of pollutants in the  raw
wastewaters of the  combined  metals data  set.   These data  are
^Sfia?±in-Ta?le? VI?-16  and  VII-17  and .  indicate  that  the?e  is
sufficient  similarity  in the raw wastes  to.  logically assume
cnmSn'T^i1?7 5f  ^ treated  pollutant  concentrations  to  the
combined  metals data base.   The  available data on these added
?£» ™?S  d° not1al}ow  homogeneity  analysis  as  was performed  on
the combined metals data base.   The  data source  for each  added
pollutant  is discussed  separately.
                               260
                                          t	

-------
Antimony (Sb) - The achievable performance for antimony is based
on data from a battery and secondary lead plant.  Both EPA sam-
pling data and recent permit data  (1978 - 1982) confirm the
achievability of 0.7 mg/1 in the battery manufacturing wastewater
matrix included in the combined data set.

Arsenic (As) - The achievable performance of 0.5 mg/1 for arsenic
is based on permit data from two nonferrous metals manufacturing
plants.  The untreated wastewater  matrix shown in Table VII-17 is
comparable with the combined data  set matrix.

Beryllium  (Be) - The treatability  of beryllium is transferred
from the nonferrous metals manufacturing industry.  The 0.3  per-
formance is achieved at a beryllium plant with the comparable
untreated wastewater matrix shown  in Table VII-17.

Mercury (Hg) - The 0.06 mg/1 treatability of mercury  is based^on
data from  four battery plants.  The untreated wastewater  matrix
at  these plants was considered  in  the  combined metals data  set.

Selenium  (Se)  - The 0.30 mg/1  treatability  of  selenium  is based
on  recent  permit data  from one  of  the  nonferrous  metals manufac-
turing plants  also used  for  antimony  performance.  The  untreated
wastewater matrix  for  this plant is shown in Table VII-17.

Silver  (Ag)  -  The  treatability  of  silver is  based on a  0.1  mg/1
treatability estimate  from the inorganic chemicals  industry.
Additional data  supporting  a treatability as  stringent  or more
stringent  than 0.1 mg/1  is  also available  from seven nonferrous
metals  manufacturing plants.   The  untreated wastewater  matrix for
 these  plants is  comparable and summarized in Table VII-17.

Thallium (Th)  -  The  0.50 nig/1 treatability  for thallium is trans-
 ferred  from the  inorganic chemicals industry.   Although no
 untreated wastewater data are available to  verify comparability
with the combined metals data set  plants,  no other sources of
 data for thallium treatability could be identified.

 Aluminum (Al)  - The 1.11 mg/1 treatability of aluminum is based
 on the mean performance of one aluminum forming plant and one
 coil coating plant.   Both of the  plants are from categories con-
 sidered in the combined metals data set, assuring untreated
 wastewater matrix comparability.

 Cobalt (Go) - The 0.05 mg/1 treatability is based on nearly com-
 plete removal of cobalt at a porcelain enameling plant with a
 mean untreated wastewater cobalt  concentration of 4.31 mg/1.  In
 this case, the analytical detection using aspiration techniques
 for this pollutant is used as the basis of the treatability.
 Porcelain enameling was considered in the combined metals data
 base, assuring untreated wastewater matrix comparability.
                                261

-------
 Fluoride  (F) - The 14.5 mg/1 treat ability  of  fluoride  is based  on
 the mean performance of an electronics and electrical  component
 manufacturing plant.  The untreated wastewater matrix  for  this
 plant shown in Table VII-17 is comparable to  the combined  metals
 data set i

 LSScF Performance
        VII-18 and VI1-19 sh°w long-term data from two plants
 which have well operated precipitation-settling treatment
 followed by filtration.  The wastewaters from both plants contain
 pollutants from metals processing and finishing operations
 ^multi-category) .   Both plants reduce hexavalent chromium before
 neutralizing and precipitating metals with lime.  A clarifier is
 nS e?_ to rem°ve much of the solids load and a filter is used to
  polish  or complete removal of suspended solids.   Plant A uses
 pressure filtration, while Plant B uses a rapid sand filter.
                                          i
 Raw waste data was collected only occasionally at  each facility
 and the raw waste  data is presented as an indication of the
 nature of the wastewater treated.  Data from Plant A was received
 as a statistical summary and is  presented as received.   Raw
 laboratory data was collected at Plant B and reviewed for spuri-
 ous points and discrepancies.  The method :of treating the data
 base is discussed  below under lime,  settle,  and filter treatment
 effectiveness.

 Table  VII-20  shows long-term data for zinc and  cadmium removal at
 muf^j0'  a Primar7 zi-nc smelter,  which operates a  LS&F system.
 This data represents about  four  months (103  data days)  taken
 immediately before the smelter was closed.   It  has  been arranged
 similarity to Plants A and  B  for  comparison  and use.

 These  data are  presented  to demonstrate  the  performance  of
 precipitation-settling-filtration (LS&F)  technology under actual
 operating conditions  and  over  a  long  period  of  time.

 It  should be noted that the iron  content  of  the  raw waste  of
 plants A  and B  is  high while that  for Plant  C is low.  This
 results,  for plants A and B, in co-precipitation of toxic  metals
WJ" ?„   ,n*  Precipitation using high-calcium lime  for pH  control
yields the results shown in Table VII-20.  Plant operating per-
 sonnel indicate that  this chemical treatment combination  (some-
times with polymer assisted coagulation) generally produces
better and more consistent  metals removal than other combinations
of sacrificial metal ions and alkalis.
                               262

-------
 The LS&F performance data presented here are based on systems
 that provide polishing filtration after effective L&S treatment.
 As previously shown, IAS treatment is equally applicable to
 wastewaters from the five categories because of the .homogene-
 ity of its raw and treated wastewaters, and other factors.
 Because of the similarity of the wastewaters after L&S treatment,
 the Agency believes these wastewaters are equally amenable to
 treatment using polishing filters added to the L&S treatment
 system.  The Agency concludes the LS&F data based on porcelain
 enameling and nonferrous smelting arid refining is directly
 applicable to the aluminum forming, copper forming, battery
 manufacturing, coil coating, and metal molding and casting
 categories, as well as to the porcelain enameling and nonferrous
 smelting and refining.

 Analysis of Treatment System Effectiveness

 Data are presented in Table VII-14 showing the mean, one day, 10-
 day  and 30-day values  for nine pollutants examined  in the LStS
 metals data base.  The mean variability factor for eight pollu-
 tants  (excluding cadmium because of  the small number of data
 points) was determined and is used to  estimate one day, 10-day,
 and 30-day values.   (The variability  factor  is the ratio  of the
 value  of concern to the mean:  the average variability factors
 are:   one  day maximum - 4.100; ten-day average -  1.821; and
 30-day average - 1.618.)  For values  not  calculated  from  the com-
 mon data base as previously  discussed,  the mean value  for pollu-
 tants  shown in Table VII-15 were multiplied  by the variability
 factors to  derive  the value  to obtain the one, ten-  and 30-day
 values.  These are  tabulated in Table VII-21.

 LSScF  technology  data are presented  in Tables VII-18  and VII-19.
 These data represent  two operating  plants (A and  B)  in which  the
 technology has been installed and  operated  for some  years.  Plant
 A data was  received as  a statistical summary and  is  presented
 without  change.  Plant  B data was  received  as raw laboratory
 analysis  data.   Discussions  with plant personnel  indicated  that
 operating  experiments and  changes  in materials and reagents  and
 occasional operating errors  had  occurred  during  the data  collec-
 tion  period.  No specific  information was available on those
 variablss.   To  sort out high values probably caused by method-
 ological  factors from random statistical  variability,  or  data
 noise, the Plant B data were analyzed. For each of the four
 pollutants (chromium, nickel,  zinc.,  and iron),  the mean and
1 standard deviation (sigma)  were calculated for the entire data
 set.   A data day was removed from the complete  data set when any
 individual pollutant concentration for that day  exceeded  the sum
 of the mean plus three  sigma for that pollutant.   Fifty-one data
 days  (from a total of about 1,300) were eliminated by this
 method.
                                 263

-------
 Another approach was also used as a check on the above method of
 eliminating certain high values.  The minimum values of raw
 wastewater concentrations from Plant B for the same four pol-
 lutants were compared to the total set of Values for the corre-
 sponding pollutants.  Any day on which the pollutant concentra-
 tion exceeded the minimum value selected from raw wastewater
 concentrations for that pollutant was discarded.  Forty- five days
 of data were eliminated by that procedure.  Forty- three days of
 data in common were eliminated by either procedures.  Since
 common engineering practice (mean plus 3 sigma) and logic
 (.treated waste should be less than raw waste) seem to coincide
 the ^ data base with the 51 spurious data days eliminated is the
 basis for all further analysis.   Range, mean, standard deviation
 and mean plus two standard deviations are shown in Tables VII-18
 and VII-19 for Cr,  Cu,  Ni, Zn,  and Fe.     ;
                                           j
 The Plant B data were separated into 1979, 1978, and total data
 base (six years)  segments.  With the statistical analysis from
 Plant A for 1978  and 1979 this  in effect created five data sets
 in which there is some  overlap  between the individual years and
 total data sets from Plant B.   By comparing these five parts it
 is apparent that  they are quite  similar and all appear to be from
 the same family of  numbers.   The largest mean found among the
 five  data sets for  each pollutant was  selected  as the long-term
 mean  for LS&F technology and is  used as the LS&F mean in Table
 V JLJLMuCJL •
Plant C  data were used  as  a  basis  for  cadmium removal  performance
and  as a check  on the zinc values  derived from plants  A and  B
The  cadmium data is  displayed  in Table VII-20 and  is incorporated
into Table VII-21 for LS&F.  The zinc  data were analyzed for com-
pliance  with the one-day and 30-day  values in Table VII-21-  no
ZiniC ^olue/°f the 103 data P°iRts  exceeded the one-day zinc  value
of 1.02  mg/1.   The 103  data  points were  separated  into blocks of
JU points and averaged.  Each  of the three full 30-day averages
was  less than the Table VII-21 value of  0.31  mg/1.  Additionally,
xr    or^nt C raw wa?tewater pollutant concentrations (Table
VII-20;  are well within the  range  of raw wastewater concentra-
tions of the combined metals data  base (Table VII-16) ,  further
supporting the  conclusion  that Plant C wastewater  data is
compatible with similar data from plants A and B.

Concentration values for regulatory  use  are displayed  in Table
VII-21.  Mean one-day,  ten-day,  and  30-day values  for  L&S for
nine pollutants were taken from  Table VII-14;  the  remaining L&S
values were developed using  the  mean values in Table VII-15 and
the mean variability factors discussed above.
                               264

-------
LSStF mean values for Cd, Cr, Ni, Zn, and Fe  are  derived  from
plants A, B, and C as discussed above.  One, ten, and 30-day
values are derived by applying the variability factor developed
from the pooled data base for the specific pollutant to  the mean
for that pollutant.  Other LSStF values  are calculated using the
long-term average or mean and the appropriate variability
factors.  Mean values for'LS&F for pollutants not already discus-
sed are derived by reducing the L&S  mean by  one-third.   The one-
third reduction was established after  examining  the percent
reduction in concentrations going from LScS to LSStF  data  for Cd,
Cr, Ni, Zn, and Fe.  The  average reduction is 0.3338 or  one-
third.

Copper levels achieved  at plants A and B may be  lower than gener-
ally achievable because of  the high  iron content and  low copper
content of the raw wastewaters.  Therefore,  the  mean concentra-
tion value  achieved is  not  used; LSStF  mean used  is  derived from
the L&S technology.

LScS cyanide mean levels shown  in Table VII-8 are ratioed to  one-
day, ten-day, and 30-day  values using  mean variability  factors.  ,
LSStF mean cyanide is calculated by  applying  the  ratios  of
removals  for L&S and LSStF as  discussed previously for LSStF ^ metals
limitations.  The cyanide performance  was  arrived at  by using the
average  metal variability factors.   The treatment method used
here is  cyanide precipitation.  Because cyanide  precipitation is
limited  by  the  same physical  processes as  the  metal precipita-
tion,  it  is  expected that the  variabilities  will be similar.
Therefore,  the  average  of the metal variability factors has been
used as  a basis  for calculating the cyanide  one-day,  ten-day, and
30-day average  treatment  effectiveness values.

The filter  performance for removing TSS as shown in Table VII-9
yields a mean effluent concentration of 2.61 mg/1 and calculates
 to a ten-day average  of 4.33,  30-day average of 3.36 mg/1; a one-
 day maximum of 8.88.   These calculated values  more than amply
 support the classic values of 10 and 15,  respectively,  which are
used for LS&F.

Although iron was  reduced in some LSStF operations, some facili-
 ties using that treatment introduce iron compounds to aid
 settling.  Therefore,  the one-day, ten-day,  and 30-day values for
 iron at LS&F were held at the LStS level so  as to not unduly
 penalize the operations which use the relatively less objection-
 able iron compounds to enhance removals of  toxic metals.
                                265

-------
 MINOR TECHNOLOGIES                       :

 Several other treatment technologies were considered for possible
 application in BPT or BAT.   These technologies are presented here
 with a full discussion for most of them.   A few are described
 only briefly because of limited technical development.

 Carbon Adsorption                        ;

 The  use of activated carbon to  remove dissolved organics from
 water and wastewater is a long  demonstrated technology.   It is
 one  of the most efficient organic removal processes available.
 This sorption process is reversible, allowing activated  carbon  to
 be regenerated for reuse by the application of heat and  steam or
 solvent.   Activated carbon has  also proved to be an effective
 adsorbent for many toxic metals,  including mercury.  Regeneration
 of carbon which has adsorbed significant  metals;  however,  may be
 difficult.

 The  term activated carbon applies to any  amorphous form  of carbon
 that has  been specially treated to give high adsorption  capaci-
 ties.   Typical raw materials include coal,  wood,  coconut shells,
 petroleum base residues,  and char from sewage sludge pyrolysis.
 A carefully controlled process  of dehydration,  carbonization, and
 oxidation yields  a product  which  4s called activated carbon.
 This  material has  a high capacity for adsorption due primarily to
 the  large surface  area available  for adsorption,  500 to  1,500
 m^/gm,  resulting  from a large number of internal  pores.   Pore
 sizes  generally range from  10 to  100 angstroms  in radius.

 Activated carbon  removes  contaminants from water by the  process
 of adsorption,  or  the attraction  and accumulation of one sub-
 stance on the surface of another.   Activated carbon preferen-
 tially adsorbs  organic compunds over other  species  and,  because
 of this  selectivity,  is  particularly effective  in removing
 organic  compounds  from aqueous  solution.

 Carbon adsorption  requires  preliminary treatment  to remove excess
 suspended solids,  oils,  and greases.   Suspended solids in  the
 influent  should be less  than 50 mg/1 to minimize  backwash
 requirements;  a downflow  carbon bed can handle  much higher levels
 (up  to 2,000  mg/1),  but requires  frequent backwashing.   Backwash-
 ing  more  than two  or three  times  a day is  not  desirable;  at 50
 mg/1 suspended  solids,  one  backwash will  suffice.   Oil and grease
 should be  less  than about 10  mg/1.   A high  level  of dissolved
 inorganic material  in  the influent  may cause problems with
 thermal  carbon  reactivation (i.e.,  scaling  and  loss of activity)
unless appropriate  preventive steps  are taken.  Such  steps might
 include pH  control,  softening, or the use  of  an acid wash  on  the
 carbon prior  to reactivation.             ;
                               266

-------
Activated carbon is available in both powdered and granular  form.
A flow diagram o£ activated carbon treatment and regeneration is
shown in figure VII-20.  A schematic of an individual adsorption
Column is shown in Figure VIIr21.  Powdered carbon is less expen-
sive per unit- weight and may have slightly higher adsorption
capacity, but it is more difficult to handle and to regenerate.

Application and Performance.  Isotherm tests have indicated  that
activated carbon is .very effective in adsorbing 65 percent of  the
SxilwgaSi pollutant! and is reasonably effective  for  another
22  percent.  Specifically, activated carbon  is very effective  in
removing 4-dlmethylphenol, fluoranthene, isophorone  naphthal-
III  all' phthalates, and phenanthrene.  Activated  carbon  is
reasonably effective on 1,1,1-trichloroethane,
1,1-dichloroethane, phenol,  and  toluene.

Table VII-22  summarizes the  treatability  effectiveness  for most
of  the  toxic  organic pollutants  by  activated carbon  as  compiled
by  EPA.  Table  VII-23  summarizes  classes  of  organic  compounds
together with samples  of  organics that  are readily adsorbed on
 carbon? Table  VII-24  lists  the effectiveness of activated carbon
 in  reaving  seven toxic organic pollutants from actual manufac-
 turing process  wastewater streams in the nonferrouS
-------
 Solid Waste Aspects:  Solid waste'from  this process  is  contami-
 nated activated carbon that requires  disposal.  Carbon  that
 undergoes regeneration reduces .the  solid waste problem  by
 reducing the frequency of carbon replacement.
           *                                ;
 Demonstration Status.  Carbon adsorption systems have been demon-
 strated to be practical and economical  in reducing COD, BOD  and
 related parameters in secondary municipal and industrial waste-
 waters; xn removing toxic or refractory organics from isolated
 industrial wastewaters;  in removing and recovering certain
 organics from wastewaters; and in the removing, and sometimes
 recovering,  Deselected inorganic chemicals from aqueous wastes.
 Carbon adsorption is a viable and economic process for  organic
 waste streams containing up to 1 to 5 percent of refractory or
 toxic organics.   Its applicability for removal of inorganics such
 as metals has also been demonstrated.

 Flotation

 Flotation is  the process  of causing particles  such as metal
 hydroxides or oil to float to the surface of a tank where they
 can be concentrated and  removed.   This is accomplished by releas-
 ing gas bubbles  which attach to the solid particles,  increasing
 their buoyancy and causing them to float.   In  principle, this
 process is the opposite  of sedimentation.   Figure VII-22 shows
 one type of flotation system.              ;

 Flotation  is  used  primarily  in  the treatment of wastewater
 streams  that  carry heavy  loads  of finely divided  suspended solids
 S£   in SoJ^d* havj-ng a  specific gravity  only slightly  greater
 than 1.0,  which would require abnormally long  sedimentation
 times, may be removed  in  much less  time  by  flotation.

 This  process may be performed in  several ways:  foam,  dispersed
 air,  dissolved air, gravity, and  vacuum  flotation  are  the  most
 commonly used techniques.  Chemical  additives  are often  used  to
 enhance  the performance of the  flotation process.

The principal difference among  types  of  flotation  is the method
 of  generating the  minute gas bubbles  (usually  air) in a  suspen-
 sion  of water and  small particles.  Chemicals  may be used  to
 improve the efficiency with any of the basic methods.  The  fol-
 lowing paragraphs  describe the different flotation techniques and
the method of bubble generation for each process.

Froth Flotation - Froth flotation is based on  differences in the
physiochemical properties in various particles.  Wettability and
surface properties affect the ability of the particles to attach
themselves to gas bubbles in an aqueous medium.  In froth flota-
tion, air is  blown through the solution containing flotation
                               268

-------
reagents.  The particles with water repellant surfaces stick to
air bubbles as they rise and are brought to the surface.  A  _
mineralized froth layer, with mineral particles attached to air
bubbles, is formed.  Particles of other minerals which are read-
ily wetted by water do not stick to air bubbles and remain in
suspension.

Dispersed Air Flotation - In dispersed air flotation  gas bubbles
are generated by introducing the air by means of mechanical agi-
tation with impellers or by forcing air through porous media.
Dispersed  air flotation is used mainly in the metallurgical
industry.

Dissolved Air Flotation - In dissolved air flotation, bubbles  are
produced by releasing air from a superstaturated solution under
relatively high pressure.  There are two types of  contact between
the gas  bubbles and particles.  The  first type is  predominant  in
the flotation of flocculated materials and involves the  entrap-
ment  of  rising gas bubbles  in the  flocculated particles^as  they
increase in size.  The bond between  the bubble and particle is
one of  physical capture only.  The second type of  contact  is  one
of adhesion.  Adhesion results  from  the intermolecular  attraction
exerted at the interface between  the solid particle  and the gase-
ous bubble.

Vacuum  Flotation - This process consists  of  saturating  the  waste-
water with air either  directly  in an aeration tank,  or  by  permit-
tine  air to enter  on the  suction  of  a  wastewater pump.   A  partial
vacuum  is  applied, which  causes  the dissolved air  to come  out of
solution as'minute bubbles.   The  bubbles  attach  to solid parti-
cles  and rise to  the  surface to form a scum blanket,  which is
normally removed by  a  skimming  mechanism.   Grit  and other  heavy
 solids  that settle to  the bottom are generally raked to_a central
 sludge  oump for  removal.   A typical vacuum flotation unit  con-^
 sists of a covered cylindrical  tank in which a partial vacuum is
maintained.   The tank  is  equipped with scum and sludge removal
 mechanisms.   The floating material is continuously swept to the
 tank periphery,  automatically discharged into a scum trough,  and
 removed from the unit  by a pump also under partial vacuum.
 Auxiliary equipment includes an aeration tank for saturating the
 wastewater with air,  a tank with a short retention time for
 removal of large bubbles, vacuum pumps, and sludge pumps.

 Application and Performance.  Flotation is used primarily in  the
 treatment of wastewater streams that carry heavy  loads ^of finely
 divided suspended solids or oil.  Solids having a specific grav-
 ity  only  slightly greater than 1.0, which would require abnor-
 mally long sedimentation times, may be removed in much less time
 by flotation.
                                269

-------
 The primary variables for flotation design are pressure, feed
 solids concentration, and retention period.  The suspended solids
 in the^effluent decrease, and the concentration of solids in the
 float increases, with increasing retention period.  When the
 flotation process is used primarily for clarification, a reten-
 tion period of 20 to 30 minutes is adequate for separation and
 concentration.

 Advantages and Limitations.   Some advantages of the flotation
 process are the high levels  of solids separation achieved in many
 applications,  the relatively low energy requirements, and the
 adaptability to meet the treatment requirements of different
 Wf5jre. tyP68 •  Limitations of flotation are that it often requires
 addition of chemicals to enhance process performance and that it
 generates large quantities of solid waste.

 Operational Factors.   Reliability:   Flotation systems normally
 are very reliable with proper maintenance of the sludge collector
 mechanism and  the motors and pumps used for aeration.

 Maintainability:   Routine maintenance is required on the pumps
 and motors.  The sludge  collector mechanism is  subject to possi-
 ble corrosion  or breakage and may require periodic replacement.

 Solid Waste Aspects:   Chemicals  are  commonly used to aid the
 flotation process  by  creating a  surface or a structure that  can
 easily  adsorb  or entrap  air  bubbles.   Inorganic chemicals,  such
 as  the  aluminum and  ferric salts,  and  activated silica,  can bind
 the particulate matter together  and  create a structure that  can
 entrap  air bubbles.   Various  organic  chemicals  can  change the
 nature  of either the  air-liquid  interface  or the solid-liquid
 interface,  or both.   These compounds usually  collect  on  the
 interface to bring about the  desired  changes.   The  added chemi-
 cals plus  the particles  in solution combine  to  form a  large  '
 volume  of sludge which must be further treated  or properly
 disposed.                                   ,              J

 Demonstration Status.  Flotation  is a  fully developed  process and
 is  readily  available  for the  treatment of  a wide variety  of
 industrial waste streams.  Dissolved air flotation  technology is
 used by can  manufacturing plants  to remove oil  and  grease in  the
wastewater from can wash lines.  It is not currently used to
 treat copper forming wastewaters.

 Centrifugation
                                            I

Centrifugation is  the  application of centrifugal force to sepa-
rate solids and liquids  in a  liquid-solid mixture or to effect
 concentration of the solids.   The application of centrifugal
force is effective because of the density differential normally
                               270

-------
found between the insoluble solids and the liquid in which they^
are contained.  As a waste treatment procedure, centrifugation in-
most often applied to dewatering of sludges.  One type of centri-
fuge is shown in Figure VII-23.

There are three common types of centrifuges:  the disc, basket,
and conveyor type.  All three operate by removing solids under
the influence of centrifugal force.  The fundamental difference
between the three types is the method by which solids are col-
lected in and discharged from the bowl.

In the disc centrifuge, the sludge feed is distributed between
narrow channels that are present as spaces between  stacked .con-
ical discs.  Suspended particles are collected and  discharged
continuously  through small orifices in the bowl wall.  The  clar-
ified effluent is discharged through an overflow weir.

A second type of centrifuge which  is useful  in dewatering sludges
is the basket centrifuge.  In  this type of  centrifuge, sludge
feed is introduced at the bottom o£ the basket, and solids  col-
lect at the bowl wall while clarified  effluent overflows  the lip
ring at the top.  Since the basket centrifuge  does  not have pro-
vision  for continuous  discharge of collected cake,  operation^
requires interruption  of the  feed  for  cake  discharge for  a  minute
or  two  in  a 10  to 30 minute overall  cycle.

The  third  type  of  centrifuge  commonly  used  in sludge dewatering
is  the  conveyor  type.  Sludge  is  fed through a stationary feed
pipe into  a  rotating bowl  in  which the solids  are settled out
against the bowl wall  by  centrifugal  force.   From the bowl  wall,
they are  moved  by a screw  to  the  end of the machine, at  which
point  they are  discharged.  The liquid effluent  is discharged
 through ports after passing the length of the bowl under cen-
trifugal  force.

Application  and Performance.   Virtually all industrial^waste
 treatment systems producing sludge can use centrifugation to
 dewater it.   Centrifugation is currently being used by a wide
 range of industrial concerns.

 The performance of sludge dewatering by centrifugation depends on
 the feed rate,  the rotational velocity of the drum, and the
 sludge composition and concentration.   Assuming proper design and
 operation, the solids content of the sludge can be increased to
 20 to 35 percent.

 Advantages and Limitations.  Sludge dewatering centrifuges have
 minimal space requirements and show a high degree  of effluent
 clarification.  The operation is  simple, clean, and relatively
                                271

-------
 inexpensive.  The area required  for a  centrifuge system  instal-
 lation is less than that required for  a filter system or sludge
 drying bed of equal capacity, and the  initial cost is lower.

 Centrifuges have a high power cost that partially offsets the low
 initial cost.  Special consideration must also be given to pro-
 viding sturdy foundations and soundproofing because of the vibra-
 tion and noise that result from centrifuge operation.  Adequate
 electrical power must also be provided since large motors are
 required.  The major difficulty encountered in the operation of
 centrifuges has been the disposal of the concentrate which is
 relatively high in suspended, non-settling solids.

 Operational Factors.   Reliability:   Centrifugation is highly
 reliable with proper control of factors such as sludge feed  con-
 sistency, and temperature.   Pretreatment such as  grit removal and
 coagulant addition may be necessary,  depending on the composition
 of the sludge and on the type of centrifuge employed.

 Maintainability:   Maintenance consists  of periodic  lubrication
 cleaning, and inspection.   The frequency and degree of inspection
 required varies  depending on the type  of sludge solids being
 dewatered and the maintenance service  conditions.   If the sludge
 is  abrasive,  it  is recommended that  the first inspection  of the
 rotating assembly be  made after appr9ximately 1,000 hours of
 operation.   If the sludge is  not abrasive  or corrosive, then the
 initial  inspection might  be  delayed.  Centrifuges not  equipped
 with  a continuous sludge  discharge system  require periodic
 shutdowns for manual  sludge  cake removal.

 Solid Waste Aspects:   Sludge  dewatered  in  the centrifugation pro-
 cess  may  be  disposed  of by landfill.  The  clarified  effluent
 Ccentrate),  if high  in dissolved or  suspended solids,  may require
 further treatment prior to discharge.      !
                                           i
 Demonstration  Status.  Centrifugation is currently used in  a
 great many commercial  applications to dewater sludge.  Work  is
 underway  to improve the efficiency, increase  the capacity  and
 lower the costs associated with  centrifugation.

 Coalescing
                                           i

The basic principle of coalescence involves  the preferential
wetting of a coalescing medium by oil droplets which accumulate
 on the medium  and then rise to the surface of the solution as
 they  combine to form larger particles.   The most important
requirements for  coalescing media are wettability for oil and
 large surface area.  Monofilament line  is sometimes used as a
coalescing medium.
                              272

-------
Coalescing stages may be integrated with a wide variety of grav-
ity oil separation devices, and some systems may incorporate
several coalescing stages.  In general, a preliminary oil skim-
ming step is desirable to avoid overloading the coalescer.

One commercially marketed system for oily waste treatment com-
bines coalescing with inclined plant separation and filtration.
In this system, the oily wastes flow into an inclined plate
settler.  This unit consists of a stack of inclined baffle plates
in a cylindrical container with an oil collection chamber at the
top.  The oil droplets rise and impinge upon the undersides of
the plants.  They then migrate upward to a guide rib that directs
the oil to the oil collection chamber, from which oil is dis-
charged for reuse or disposal.

The oily water continues on through another cylinder containing
replaceable filter cartridges that remove suspended particles^
from the waste.  From there the wastewater enters a final cylin-
der in which the coalescing material is housed.  As the  oily
water passes through the many small, irregular, continuous
passages  in the coalescing material, the oil droplets coalesce
and rise  to an oil collection chamber.

Application and Performance.  Coalescing is used to treat oily
wastes  that do not separate readily  in  simple  gravity systems.
The three stage system described above has achieved effluent
concentrations of 10 to 15 mg/1 oil  and  grease from raw  waste
concentrations of 1,000 mg/1 or more.

Advantages  and Limitations.  Coalescing  allows removal  of oil
droplets  too  finely  dispersed  for  conventional gravity
separation-skimming  technology.  It  also  can significantly  reduce
the residence  times  (and  therefore  separator volumes) required  to
achieve separation of oil  from  some  wastes.  Because  of  its  sim-
plicity,  coalescing  provides  generally  high  reliability  and low
capital and operating costs.  Coalescing  is  not generally^effec-
tive  in removing  soluble  or  chemically  stabilized  emulsified
oils.   To avoid  plugging,  coalescers  must be protected  by  pre-
treatment from the very high  concentrations  of free  oil and
grease  and  suspended solids.   Frequent  replacement  of prefilters
may be  necessary  when raw waste oil concentrations  are  high.

Operational Factors.  Reliability:   Coalescing is  inherently ,
highly  reliable  since  there  are no moving parts and  the coalesc-
 ing substrate (monofilament,  etc.)  is inert in the process and
therefore not subject  to  frequent  regeneration or  replacement
 requirements.   Large loads or inadequate preliminary^treatment;
however, may  result  in plugging or bypass of coalescing stages.
                               273

-------
 Maintainability:   Maintenance requirements are generally limited
 to replacement of the coalescing medium on an infrequent basis.
 Solid Waste Aspects:
 this process.
            No appreciable  solid waste is generated by
 Demonstration Status.   Coalescing has been fully demonstrated in
 industries  generating  oily wastewater.   A few are known to be in
 use at copper forming  plants.

 Cyanide Oxidation by Chlorine

 Cyanide oxidation using chlorine is  widely used in industrial
 waste  treatment  to oxidize cyanide.   Chlorine can be  utilized in
 either the  elemental or hypochlorite forms.   This classic proced-
 ure can be  illustrated by  the  following  two step chemical reac-
 tion:
NaCN + 2NaOH
2.  3C12 + 6NaOH + 2NaCNO
                                    2NaCl
                    2NaHC03
                                              6NaCl +  2H20
The  reaction presented  as  equation  (2)  for  the  oxidation  of  cya-
nate is the final step  in  the oxidation of  cyanide.  A complete
system for the alkaline chlorination  of cyanide is  shown  in
Figure VII-24.

The alkaline chlorination  process oxidizes  cyanides to carbon
dioxide and nitrogen.   The equipment  often  consists of an equali-
zation tank followed by two reaction  tanks, although the  reaction
can be carried out in a single tank.  Each  tank has an electronic
recorder-controller to  maintain required conditions with  respect
to pH^and oxidation reduction potential (ORP) .   In  the first
reaction tank, conditions  are adjusted  to oxidize cyanides to
cyanates.  To effect the reaction, chlorine is  metered to the
reaction tank as required  to maintain the ORP in the range of 350
to 400 millivolts, and  50  percent aqueous caustic soda is added
to maintain a pH range  of  9.5 to 10.  In the second reaction
tank, conditions are maintained to oxidize cyanate  to carbon
dioxide and nitrogen.   The desirable ORP and pH  for this  reaction
are 600 millivolts and  a pH of 8.0.  Each of the reaction tanks
is equipped with a propeller agitator designed to provide approx-
imately one turnover per minute.  Treatment by  the batch  process
is accomplished by using two tanks, one for collection of water
over a specified time period, and one tank for  the treatment of
an accumulated batch.   If  dumps of concentrated wastes are fre-
quent,  another tank may  be required to  equalize  the flow  to the
treatment tank.   When the holding tank  is full,   the liquid is
transferred to the reaction tank for treatment.   After treatment,
the supernatant is discharged and the sludges are collected for
removal and ultimate disposal.
                               274

-------
Application and Performance.  The oxidation of cyanide waste by
chlorine is a classic process and is found in most industrial
plants using cyanide.  This process is capable of achieving
effluent levels of free cyanide that are nondetectable.  The
process is potentially applicable to aluminum forming facilities
where cyanide is a component in conversion coating formulations
or is added as a corrosion  inhibitor in heat treatment opera-
tions.

Advantages and Limitations.  Some advantages of chlorine•oxidaton
for handling process effluents are operation at ambient tempera-
ture, suitability for automatic control, and low cost.  Disadvan-
tages include the need for  careful pH control, possible chemical
interference in the treatment of mixed wastes, and the potential
hazard of  storing and handling chlorine gas.  If organic com-
pounds are present, toxic chlorinated organics may be generated.
Alkaline chlorination is not effective in treating metallocyanide
complexes, such as the ferrocyanide.

Operational Factors.  Reliability:  Chlorine oxidation is  highly
reliable with proper monitoring and control, and proper pretreat-
ment  to control interfering substances.

Maintainability:  Maintenance consists of periodic removal of
sludge and recalibration of instruments.

Solid Waste Aspects:  There is no  solid waste problem associated
with  chlorine oxidation.

Demonstration Status.  The  oxidation of  cyanide wastes by  chlo-
rine  is  a  widely used process  in  plants  using cyanide in cleaning
and metal  processing baths.

Cyanide Oxidation by Ozone               .

Ozone is a highly reactive  oxidizing agent  which  is  approximately
10 times more  soluble  than  oxygen on  a weight basis  in water.
Ozone may  be produced by several  methods, but the  silent electri-
cal  discharge  method is  predominant  in the  field.   The silent
electrical discharge process  produces  ozone by  passing oxygen  or
air between electrodes  separated  by  an insulating material. A
complete  ozonation  system  is  represented in Figure VII-25.

Application and Performance.   Ozonation  has been  applied commer-
 cially to  oxidize  cyanides, phenolic  chemicals,  and organometal
 complexes.  Its applicability to  photographic wastewaters  has
been studied in the laboratory with good results.   Ozone is used
 in industrial  waste treatment primarily  to  oxidize cyanide to
 cyanate and to oxidize  phenols and dyes  to  a variety of colorless
 nontoxic products.
                                275

-------
 Oxidation of cyanide to cyanate is illustrated below:

      CN" + 03 —«- CNCT + 02

 Continued exposure to ozone will convert the cyanate formed to
 carbon dioxide  and ammonia; however,  this is not economically
 practical.

 Ozone oxidation of cyanide to cyanate requires 1.8 to 2.0 pounds
 ozone per pound of CN~;  complete oxidation requires 4,6 to 5.0
 pounds ozone per pound of CN~.   Zinc, copper,  and nickel cya-
 nides are easily destroyed to a nondetectable  level, but cobalt
 and iron cyanides are more resistant  to ozone  treatment.

 Advantages  and  Limitations.  Some advantages of ozone oxidation
 for handling process effluents  are its suitability to automatic
 control and on-site generation and the fact that reaction prod-
 ucts are not chlorinated organics and no dissolved solids are
 added in the treatment step.   Ozone in the presence of activated
 carbon,  ultraviolet,  and other  promoters shows promise of reduc-
 ing reaction time and improving ozone utilization, but the
 process  at  present  is limited by high capital  expense,  possible
 chemical interference in the treatment of mixed wastes,  and an
 energy requirement  of 25 kwh/kg of ozone generated.   Cyanide is
 not economically  oxidized with  03 beyond the cyanate form.

 Operational Factors.   Reliability:  Ozone oxidation is  highly
 reliable with proper monitoring and control, and proper prelimi-
 nary treatment  to control interfering substances.

 Maintainability:  Maintenance consists of periodic removal of
 sludge,  and periodic  renewal  of filters  and desiccators  required
 for the  input of  clean dry air;  filter life is a function of
 input  concentrations  of  detrimental constituents.

 Solid  Waste Aspects:   Preliminary treatment to eliminate sub-
 stances  which will  interfere  with the process  may  be necessary.
 Dewatering  of sludge  generated  in the ozone oxidation process  or
 in  an  in-line  process  may be  desirable  prior to  disposal.

 Cyanide  Oxidation by  Ozone  with UV  Radiation

One  of the  modifications  of the ozonation process  is  the simulta-
neous  application of  ultraviolet  light and  ozone for  the treat-
ment of  wastewater, including treatment  of  halogenated organics.
The  combined  action of these  two  forms produces reactions by
photolysis, photosensitization, hydroxylation,   oxygenation, and
oxidation.  The process  is  unique because several  reactions and
reaction species are  active simultaneously.
                              276

-------
Ozonation is facilitated by ultraviolet absorption because both
the ozone and the reactant molecules are raised to a higher
energy state so that they react more rapidly.  In addition, free
radicals for use in the reaction are readily hydrolyzed by the
water present.  The energy and reaction intermediates created by
the introduction of both ultraviolet and ozone greatly reduce the
amount of ozone required compared with a system using ozone
alone.  Figure VII-26 shows a three-stage UV-ozone system.  A
system to treat mixed cyanides requires preliminary treatment
that involves chemical coagulation, sedimentation, clarification,
equalization, and pH adjustment.

Application and Performance.  The ozone-UV radiation process was
developed primarily for cyanide treatment in the electroplating
and color photo-processing areas.  It has been successfully
applied to mixed cyanides and organics from organic chemicals
manufacturing processes.  The process is particularly useful for
treatment of complexed cyanides such as ferricyanide, copper
cyanide, and nickel cyanide, that are resistant to ozone.

Demonstration Status.  Ozone combined with UV radiation is a
relatively new technology.  Four units^are currently in operation
and all four treat cyanide-bearing waste although none are used
at copper forming plants.

Cyanide Oxidation by Hydrogen Peroxide

Hydrogen peroxide oxidation removes both cyanide and metals in
cyanide-containing wastewaters.  In this process, cyanide-bearing
waters are heated to 49°C to 54°C  (120°F to 130°F) and the pH is^
adjusted to 10.5 to 11.8.  Formalin  (37 percent formaldehyde) is
added while the tank is vigorously agitated.- After two to five
minutes, a proprietary peroxygen compound  (41 percent hydrogen
peroxide with a catalyst and additives) is added.  After  an hour
of mixing, the reaction is  complete.  The  cyanide is converted to
cyanate and the metals are precipitated as oxides or hydroxides.
The metals are then removed  from solution  by  either settling or
filtration.

The main equipment required  for this process  is two holding tanks
equipped with heaters  and  air  spargers  or  mechanical stirrers.
These tanks may be used in  a batch or continuous  fashion, with
one  tank being used  for treatment  while  the  other is being
filled.  A settling tank or  a  filter is needed  to concentrate the
precipitate.

Application  and Performance.   The  hydrogen peroxide  oxidation
process  is applicable  to  cyanide-bearing wastewaters,  especially
those containing  metal-cyanide complexes.  In terms  of waste
reduction performance,  this  process  can reduce  total  cyanide  to
                                277

-------
 less than 0.1  mg/1 and the zinc or cadmium concentrations to less
 than 1.0 mg/1.
                                           !
 Advantages and Limitations.   Chemical costs  are similar to those
 for alkaline chlorination using chlorine and lower than those for
 treatment with hypochlorite.   All free cyanide  reacts  and is com-
 pletely oxidized to the less  toxic cyanate state.   In  addition,
 the metals precipitate and settle quickly, and  they may be recov-
 erable  in many instances;  however, the process  requires energy
 expenditures to heat the wastewater prior to treatment.

 Demonstration  Status.   This treatment process was  introduced in
 1971 and is used in several facilities.   Np  copper forming plants
 use oxidation  by hydrogen peroxide.
                                           i
 Evaporation

 Evaporation is  a concentration process.   Water  is  evaporated from
 a  solution,  increasing the concentration of  solute in  the remain-
 ing solution.   If the  resulting water vapor  is  condensed back to
 liquid  water,  the evaporation-condensation process is  called dis-
 tillation.   However, to be consistent with industry terminology,
 evaporation is  used in this report to describe  both processes.
 Both atmospheric and vacuum evaporation  are  commonly used in
 industry today.   Specific  evaporation techniques are shown in
 Figure  VII-27 and discussed below.  •
                                           I
 Atmospheric  evaporation could  be  accomplished simply by  boiling
 the liquid.  To aid evaporation,  heated  liquid  is  sprayed on an
 evaporation  surface, and air is blown over the  surface  and subse-
 quently released to the atmosphere.   Thus, evaporation.occurs  by
 humidification  of the  air  stream,  similar to  a  drying process.
 Equipment  for carrying out atmospheric evaporation is quite
 similar for  most  applications.  The  major element  is generally a
 Jacked  column with an  accumulator bottom.  Accumulated wastewater
 s pumped  from  the  base  of the column, through  a, heat exchanger,
 and  back into the top  of the column,  where it is sprayed into  the
 packing.  At the  same  time, air drawn upward  through the  packing
 by  a fan is heated  as  it contacts  the hot liquid.   The  liquid
 partially vaporizes  and  humidifies the air stream.  The  fan  then
 blows the hot,  humid air to the outside  atmosphere.  A  scrubber
 is often unnecessary because the packed  column  itself acts  as a
 scrubber.
                                           j
Another form of atmospheric evaporator also works  on the  air
humidification  principle,  but  the  evaporated water  is recovered
 for  reuse by condensation.  These  air humidification techniques
 operate well below  the boiling point  of water and  can utilize
waste process heat  to  supply the  energy  required.
                               278

-------
In vacuum evaporation, the evaporation pressure is lowered to
cause the liquid to boil at reduced temperatures.  All of^the
water vapor is condensed and, to maintain the vacuum condition,
noncondensible gases  (air in particular) are removed by a vacuum
pump.  Vacuum evaporation may be either single or double effect.
In double effect evaporation, two evaporators are used, and the
water vapor from the  first evaporator (which may be heated by
steam) is used to supply heat to the second evaporator.  As it
supplies heat, the water vapor from the first evaporator con-
denses.  Approximately equal quantities of wastewater are evapo-
rated in each unit; thus, the double effect system evaporates
twice the amount of water that a single effect system does, at
nearly the 'same cost  in energy but with added capital cost and
complexity.  The double effect technique is thermodynamically
possible because the  second evaporator is maintained at lower
pressure (higher vacuum) and, therefore, lower evaporation tem-
perature.  Another means of increasing energy efficiency is vapor
recompression  (thermal or mechanical), which enables heat to be
transferred from the  condensing water vapor to the evaporating
wastewater.  Vacuum evaporation equipment may be classified as
submerged tube or climbing film evaporation units.

In  the most commonly  used submerged tube evaporator, the heating
and condensing coil are contained  in a single vessel to reduce
capital  cost.  The vacuum in  the vessel  is maintained by  an
eductor-type pump, which creates the required vacuum by the flow
of  the condenser cooling water through a venturi.  Wastewater
accumulates in the bottom of  the vessel, and  it  is evaporated by
means  of submerged  steam  coils.  The resulting water vapor  con-
denses as it contacts the condensing coils in the  top of^the
vessel.  The  condensate then  drips off  the condensing  coils  into
a collection trough that  carries   it out of the  vessel.   Con-
centrate is removed  from  the  bottom of  the vessel.

The major  elements  of the climbing film evaporator are  the  evapo-
rator, separator,  condenser,  and vacuum pump.  Wastewater is
 "drawn"  into  the  system by  the vacuum  so that a constant  liquid
 level is maintained  in the  separator.  Liquid enters  the  steam-
 jacketed evaporator tubes,  and part, of  it  evaporates  so that  a
 mixture  of  vapor  and  liquid  enters the  separator.  The  design of
 the separator is  such that  the  liquid  is continuously  circulated
 from the separator to the evaporator.   The  vapor entering the
 separator  flows  out through a mesh entrainment  separator to the
 condenser,  where  it is condensed as it  flows  down through the
 condenser tubes.   The condensate,  along with any entrained air,
 is pumped  out of the bottom of  the condenser by a liquid ring
 vacuum pump.   The liquid seal provided by the condensate keeps
 the vacuum in the system from being broken.
                                279

-------
Application and Performance.   Both atmospheric and vacuum
evaporation are used in many, industrial plants,  mainly for the
concentration and recovery of process solutions.   Many of these
evaporators also recover water for rinsing.   Evaporation has also
been applied to recovery of phosphate metal-cleaning solutions.

In th'eory,  evaporation should yield a concentrate and a deionized
condensate.   Actually,  carry-over has resulted in coridensate
metal  concentrations as high  as  10 mg/1,  although the usual level
is  less than 3  iag/1,  pure enough for most final  rinses.   The con-
densate may also contain organic brighteners  and antifoaming
agents.  These  can be removed with an activated  carbon bed,  if
necessary.   Samples  from one  plant showed 1,900  mg/1 zinc in the
feed,  4,570 mg/1 in  the concentrate,  and  0.4  mg/1 in the condens-
ate.   Another plant  had 416 mg/1 copper in the feed and 21,800
mg/1 in the concentrate.   Chromium analysis  for  that plant indi-
cated  5,060 mg/1 in  the feed  and 27,500 mg/1  in  the concentrate.
Evaporators  are available in  a range of capacities,  typically
from 15 to  75 gph, and  may be used in parallel arrangements  for
processing  of higher flow rates.

Advantages  and  Limitations.   Advantages of the evaporation pro-
cess ^ are that it permits  recovery of a wide variety of process
chemicals,  and  it  is  often applicable to  concentration or removal
of  compounds  which cannot be  accomplished by  any  other means.
The major disadvantage  is that the evaporation process consumes
relatively  large amounts  of energy for the evaporation of water.
The recovery  of waste heat from  many  industrial processes (e.g.,
diesel generators, incinerators,  boilers,  and furnaces)  should be
considered  as a source  of this heat  for a totally integrated
evaporation system.   Also,  in some cases  solar heating could be
inexpensively and  effectively applied to  evaporation units.   For
some applications, preliminary treatment  may  be required to
remove solids or bacteria which  tend  to cause fouling in the
condenser or  evaporator.   The buildup of  scale on the evaporator
surfaces reduces the  heat transfer efficiency and may present  a
maintenance problem  or  increase  operating 'cost.   It  has  been
demonstrated that  fouling of  the heat transfer surfaces  can  be
avoided or minimized  for1  certain  dissolved solids  by maintaining
a seed slurry which provides  preferential  sites for  precipitate
deposition.  In addition,  low temperature differences  in the
evaporator will  eliminate nucleate boiling and supersaturation
effects.  Steam distillable impurities  in the process  stream are
carried over with the product  water and must  be handled  by
preliminary or  post  treatment.             '.
                                           \
Operational Factors.   Reliability:  Proper maintenance will
ensure a high degree  of reliability for the system.  Without such
attention,  rapid fouling  or deterioration  of  vacuum  seals may
occur, especially when handling corrosive  liquids.
                               280

-------
Maintainability:  Operating parameters can be automatically
controlled.  Preliminary treatment may be required, as well as
periodic cleaning of the system.  Regular replacement of seals,
especially in a corrosive environment, may be necessary.

Solid Waste Aspects:  With only a few exceptions, the process
does not generate appreciable quantities of solid waste.

Demonstration Status.  Evaporation is a fully developed, com-
mercially available wastewater treatment system.  It is used
extensively to  recover plating chemicals in the  electroplating
industry and a pilot scale unit has been used in connection with
phosphating of  aluminum.  Proven performance in  silver  recovery
indicates that  evaporation could be a useful treatment  operation
for the photographic industry, as well as for metal finishing.

Gravity Sludge ^Thickening

In the gravity  thickening process, dilute sludge is fed from  a
primary settling tank or clarifier to a thickening tank where
rakes stir the  sludge gently  to densify it and to push  it  to  a
central collection well.  The supernatant is returned to the
primary settling tank.  The thickened sludge that  collects on the
bottom of the tank is pumped  to dewatering equipment or hauled
away.  Figure VII™28 shows the  construction of a gravity
thickener.

Application and Performance.  Thickeners are generally  used in
facilities where the sludge is  to be  further dewatered  by  a com-
pact mechanical device  such as  a vacuum filter or  centrifuge.
Doubling  the  solids  content in  the  thickener substantially
reduces capital and  operating cost  of the subsequent dewatering
device and also reduces  cost  for hauling.  The process  is
potentially applicable  to  almost any  industrial  plant.

Organic sludges from sedimentation  units  of 1 to 2  percent solids
concentration can usually  be  gravity  thickened  to  6  to  10  per-
cent;  chemical  sludges  can be thickened to 4 to  6  percent.

Advantages and  Limitations.   The principal  advantage  of a  gravity
 sludge thickening process  is  that  it:  facilitates further sludge
dewatering.   Other  advantages are high  reliability and  minimum
maintenance  requirements.

Limitations  of the  sludge  thickening  process  are its  sensitivity
 to the flow  rate  through the  thickener  and  the^sludge  removal
 rate.   These rates  must be low  enough not to  disturb the
 thickened sludge.
                                281

-------
 Operational Factors.  Reliability:  Reliability is high with
 proper design and operation.  A gravity thickener is designed on
 the basis of square feet per pound of solids per day, in which
 the required surface area is related to the solids entering and
 leaving the unit.  Thickener area requirements are also expressed
 in terms of mass loading, kilograms of solids per sqxiare meter
 per day (Ibs/sq ft/day).

 Maintainability:  Twice a year, a thickener must be shut down for
 lubrication of the drive mechanisms.  Occasionally, water must be
 pumped back through the system in order to clear sludge pipes.

 Solid Waste Aspects:  Thickened sludge from a gravity thickening
 process will usually require further dewatering prior to dispo-
 sal,  incineration, or drying.   The clear effluent may be recircu-
 lated in part,  or it may be subjected to further treatment prior
 to discharge.

 Demonstration Status.   Gravity sludge thickeners are used
 throughout  industry to reduce  sludge water content to a level
 where the sludge may be efficiently handled.   Further dewatering
 is  usually  practiced to minimize costs of hauling the sludge to
 approved landfill areas.
Ion Exchange                              ,

Ion exchange  is  a  process  in which ions,  held by  electrostatic
forces to  charged  functional groups  on  the  surface  of  the  ion
exchange resin,  are  exchanged  for ions  of similar charge  from the
solution in which  the resin  is  immersed.  This  is classified  as  a
sorption process because the exchange occurs  on the surface of
the resin, and the exchanging  ion must  undergo  a  phase transfer
from solution phase  to  solid phase.  Thus,,  ionic  contaminants in
a waste stream can be exchanged  for  the harmless  ions  of the
resin.
                                          j
Although the  precise technique may vary slightly  according to the
applzcation involved, a generalized  process description follows.
The wastewater stream being  treated  passes  through  a filter to
remove any solids, then flows through a cation  exchanger which
contains the  ion exchange  resin.   Here, metallic  impurities such
as copper, iron, and trivalent chromium are retained.   The stream
then passes through the anion exchanger and its assocaited resin.
Hexavalent chromium  (in the  form  of  chromate  or dichromate),  for
example, is retained in this stage.  If one pass  does  not  reduce
the contaminant  levels sufficiencly, the  stream may  then enter
another series of  exchangers.  Many  ion exchange  systems are
equipped with more than one  set of exchangers for this  reason.
                               282

-------
The other major portion of the ion exchange process concerns the
regeneration of the resin, which now holds those impurities
retained from the waste stream.  An ion exchange unit with
lii-place-regeneration is shown in Figure VII-29.  Metal ions such
as nickel are removed by an acid, cation exchange resin, which  is
regenerated with hydrochloric or sulfuric acid, replacing the
metal ion with one or more hydrogen ions.  Anions such as dichro-
mate are removed by a basic anion exchange resin, which is regen-
erated with sodium hydroxide, replacing the anion with one or
more hydroxyl ions.  The three principal methods employed by
industry for regenerating the spent resin are:

     (A)  Replacement Servicer-.. A regeneration service replaces
          the spent resin with regenerated resin, and regenerates
          the spent resin at  its own  facility.  The service  then
          has the problem of  treating and disposing of the spent
          regenerant.

      (B)  In-Place Regeneration:  Some establishments may  find it
          less expensive  to do  their  own regeneration.  The  spent
          resin  column  is  shut  down for perhaps an hour,  and the
          spent  resin  is  regenerated. * This  results in  one  or
          more waste  streams  which  must be  treated in an appro-
          priate manner.  Regeneration is performed as  the  resins
          require it,  usually every few months.

      (C)  Cyclic Regeneration:   In this process,  the regeneration
          of the spent resins takes place within the ion exchange
          unit itself in alternating cycles with the ion removal
          process.   A regeneration frequency of twice an hour^is
           typical.   This very short cycle time permits operation
          with a very small quantity of resin and with fairly
           concentrated solutions,  resulting in a very compact
           system.  Again, this process varies according to^appli-
           cation, but the regeneration cycle generally begins
           with caustic being pumped through the anion exchanger,
           carrying out hexavalent chromium, for example, as
           sodium dichromate.  The sodium dichromate stream then
           passes through a cation exchanger, converting the
           sodium dichromate to chromic acid.  After concentration
           by evaporation or other means, the  chromic acid can  be
           returned to the process line.  Meanwhile, the cation
           exchanger is regenerated with sulfuric acid, resulting
           in a waste acid stream containing the metallic impuri-
           ties  removed earlier.  Flushing the  exchangers with
           water completes the cycle.  Thus, the wastewater  is
           purified and, in this example, chromic acid is recov-
           ered.  The ion exchangers,  with newly regenerated
           resin, then  enter  the ion  removal cycle  again.
                                283

-------
Application and Performance.   The  list  of  pollutants  for  which
the ion exchange  system has proven effective  includes  aluminum,
arsenic, cadmium,  chromium  (hexavalent  and trivalent),  copper,
cyanide, gold, iron,  lead, manganese, nickel,  selenium, silver,
tin, zinc, and others.  Thus,  it can be applied  to  a wide variety
of industrial concerns.  Because of the heavy concentrations  of
metals in their wastewater, the metal finishing  industries util-
ize ion exchange  in several ways.   As an end-of-pipe treatment,
ion exchange is certainly feasible,  but its greatest value is  in
recovery applications.  It is  commonly  used as an integrated
treatment to recover  rinse water and process  chemicals.   Some
electroplating facilities use  ion  exchange to concentrate and
purify plating baths.  Also, many  industrial  concerns,  including
a number of aluminum  forming plants, use ion  exchange  to  reduce
salt concentrations in incoming water sources.
                                           i

Ion exchange is highly efficient at recovering metal-bearing
solutions.  Recovery  of chromium,  nickel,  phosphate solution,  and
sulfuric acid from anodizing is common.  A chromic  acid recovery
efficiency of 99.5 percent has been demonstrated.  Typical data
for purification  of rinse water are displayed in Table VII-25.
                                  •
Advantages and Limitations.  Ion exchange  is  a versatile  technol-
ogy applicable to  a great many situations.  This flexibility,
along with its compact nature  and  performance, makes ion  exchange
a very effective  method of wastewater treatment.  However,  the
resins in these systems can prove  to be a  ^limiting  factor.  The
thermal limits of  the ariion resins,  generally in the vicinity  of
60 C, could prevent its use in certain  situations.  Similarly,
nitric acid, chromic  acid, and hydrogen peroxide can all  damage
the resins, as will iron, manganese, and copper when present with
sufficient concentrations of dissolved  oxygen.  Removal of a par-
ticular trace contaminant may be uneconomical because  of  the
presence of other  ionic species that are preferentially removed.
The regeneration  of the resins presents its own  problems.   The
cost of the regenerative chemicals  can  be  high.  In addition,  the
waste streams originating from the  regeneration process are
extremely high in pollutant concentrations, although low  in
volume.  These must be further processed for  proper disposal.

Operational Factors.  Reliability:  With the  exception of occa-
sional clogging or fouling of the resins,  ion exchange has  proved
to be a highly dependable technology.      '

Maintainability:   Only the normal maintenance of pumps, valves,
piping, and other hardware used in  the  regeneration process is
required.
                                           I
Solid Waste Aspects:  Few, if any,  solids  accumulate within the
ion exchangers, and those which do  appear  are removed by  the
                               284

-------
regeneration process.  Proper prior treatment and planning can
eliminate solid buildup problems altogether.  The brine resulting
from regeneration of the ion exchange resin most usually must be
treated to remove metals before discharge.  This can generate
solid waste.

Demonstration Status.  All of the ion exchange applications
discussed in this section are in commercial use, and industry
sources estimate the number of ion exchange units currently in
the field at well over 120.  The research and development in ion
exchange is focusing on improving the quality and efficiency of
the resins, rather than new applications.  Work is also being
done on a continuous regeneration process whereby the resins are
contained on a fluid- transfusible belt.  The belt passes through
a compartmented tank with ion exchange, washing, and regeneration
sections.  The resins are therefore continually used and
regenerated.  No such system, however, has been reported beyond
the pilot stage.

Insoluble Starch Xanthate

Insoluble starch xanthate is essentially  an ion exchange medium
used to remove dissolved heavy metals from wastewater.  The water
may then either be reused  (recovery application) or discharged
 (end-of-pipe application).  In a  commercial electroplating
operation,  starch xanthate is coated on a filter medium.  Rinse
water  containing dragged  out heavy metals is  circulated through
the filters and then reused for rinsing.  The starch-heavy metal
 complex  is  disposed  of  and replaced periodically.  Laboratory
tests  indicate'that  recovery of metals  from the complex is
 feasible, with regeneration of  the  starch xanthate.  Besides
electroplating, starch  xanthate is potentially  applicable to
 aluminum forming,  coil  coating, porcelain enameling, copper
 fabrication, and any other industrial plants  where  dilute^metal
wastewater  streams  are  generated.   Its  present  use  is  limited  to
 one electroplating  plant.

 Peat Adsorption

 Peat moss  is a complex  natural  organic  material containing  lignin
 and  cellulose  as  major  constituents.' These constituents,  partic-
 ularly lignin, bear polar functional  groups,  such as  alcohols,
 aldehydes,  ketones,  acids,  phenolic hydroxides,  and ethers,  that
 can be involved in chemical bonding.  Because of the  polar  nature
 of the material,  its adsorption of dissolved solids^such_as
 transition metals  and  polar  organic molecules is  quite high.
 These properties  have  led to  the use of peat as an agent for the
 purification of industrial wastewater.
                                285

-------
Peat adsorption is  a "polishing" process which can achieve very
low  effluent  concentrations  for several pollutants.   If the con-
centrations of pollutants  are above 10  mg/1,  then peat: adsorption
must be  preceded by pH adjustment for metals  precipitation and
subsequent clarification.  Pretreatment is also required for
chromium wastes using ferric chloride and sodium sulfide.   The
wastewater is then  pumped  into a large  metal  chamber called a
kier which contains a layer  of peat through which the waste
stream passes.   The water  flows to a second kier for further
adsorption.   The wastewater  is then ready for discharge.   This
system may be automated or manually operated.
                                           I
Application and Performance.   Peat adsorption can be used in
copper forming plants for  removal of residual dissolved metals
from clarifier effluent.   Peat moss may be used to treiat waste-
waters containing heavy metals such as  mercury,  cadmium,  zinc,
copper,  iron,  nickel,  chromium,  and lead,  as  well as organic
matter such as  oil,  detergents,  and dyes.   Peat adsorption is
currently used commercially  at a textile plant,  a newsprint
facility, and a metal reclamation operation.

Table VII-26  contains performance figures  obtained from pilot
plant studies.   Peat adsorption was preceded  by pH adjustment  for
precipitation and by clarification.

In addition,  pilot  plant studies have shown that chelated  metal
wastes,  as well as  the chelating agents themselves,  are removed
by contact with peat moss.

Advantages and  Limitations.   The major  advantages  of the  system
include  its ability to yield low pollutant concentrations,  its
broad scope in  terms  of the  pollutants  eliminated,  and its  capac-
ity  to accept wide  variations of wastewater composition.

Limitations include the cost of  purchasing,! storing,  and  dispos-
ing  of the peat  moss;  the  necessity for regular  replacement of
the  peat may  lead to high  operation and maintenance  costs.   Also,
the  pH adjustment must  be  altered according to  the composition of
the  waste stream.
                                           I
Operational Factors.  Reliability:   The question of  long-term
reliability is not  yet  fully  answered.  Although the manufacturer
reports  it to be a  highly  reliable system,  operating experience
is needed to verify  the claim.

Maintainability:  The peat moss  used in this process  soon
exhausts its  capacity  to adsorb  pollutants.  At  that time,  the
kiers  must be opened, the  peat removed,  and; fresh  peat  placed
inside.  Although this  procedure is  easily and  quickly  accom-
plished,  it must be  done at  regular  intervals, or  the  system's
efficiency drops  drastically.
                               286

-------
Solid Waste Aspects:  After removal from the kter, the spent peat
must be eliminated.  If incineration is used, precautions should
be taken to ensure that those pollutants removed from the water
are not released again in the combustion process.  Presence of
sulfides in the spent peat, for example, will give rise to sulfur
dioxide in the fumes from burning.  The presence of significant
quantities of toxic heavy metals in copper forming wastewater
will in general preclude incineration of peat used in treating
these wastes.

Demonstration Status.  Only three facilities currently use
commercial adsorption systems in the United States - a textile
manufacturer, a newsprint facility, and a metal reclamation firm.
No data have been reported showing the use of peat adsorption in
copper forming plants.

Membrane Filtration

Membrane filtration is a treatment system for removing precipi-
tated metals from a wastewater stream.  It must therefore be
preceded by those treatment techniques which will properly pre-
pare the wastewater for solids removal.  Typically, a membrane
filtration unit is preceded by pH adjustment or sulfide addition
for precipitation of the metals.  These steps are followed by the
addition of a proprietary chemical reagent which  causes the pre-
cipitate to be non-gelatinous, easily dewatered, and highly
stable.  The resulting mixture of pretreated wastewater and
reagent is continuously recirculated through a filter module and
back  into a recirculation tank.  The filter module contains tubu-
lar membranes.  While the reagent-metal hydroxide precipitate
mixture flows through the inside  of the tubes, the water  and any
dissolved salts permeate the membrane.  When the  recirculating_
slurry reaches a concentration of 10 to 15 percent solids, it is
pumped out of the  system as sludge.

Application and Performance.  Membrane  filtration appears to be
applicable to any  wastewater or process water containing  metal
ions  which can be  precipitated using hydroxide, sulfide,  or car-
bonate precipitation.  It  could function  as  the primary  treatment
system, but also might find application as a polishing treatment
 (after precipitation  and settling) to  ensure continued compliance
with  metals  limitations.  Membrane filtration systems are being
used  in a number of industrial applications, particularly in the
metal finishing area.  They have  also been used  for heavy metals
removal in  the metal  fabrication  industry and the paper  industry.

The permeate is  claimed by  one manufacturer  to  contain less,than
the effluent  concentrations shown in Table VII-27, regardless of
the influent  concentrations.  These  claims have  been  largely  sub-
stantiated  by the  analysis  of water samples  at various plants in
various  industries.
                                287

-------
 In the performance predictions for this technology, pollutant
 concentrations are reduced to the levels shown in Table VII-27
 unless lower levels are present in the influent stream.
                                          i
 Advantages and Limitations.   A major advantage of the membrane
 filtration system is that installations can use most of the
 conventional end-of-pipe systems that may already be in place.
 Removal efficiencies are claimed to be excellent, even with sud-
 den variation of pollutant input rates; however, the effective-
 ness of the membrane filtration system can  be limited by clogging
 of the filters.   Because pH  changes in the  waste stream greatly
 intensify clogging problems,  the pH must be carefully monitored
 and controlled.   Clogging can force the shutdown of the system
 and^may interfere with production.   In addition, relatively high
 capital cost of this system  may limit its iuse.

 Operational Factors.   Reliability:   Membrane filtration has been
 shown to be a very reliable  system,  provided that the pH is
 strictly controlled.   Improper pH can result in the clogging of
 the membrane.  Also,  surges  in the  flow rate of the waste stream
 must be controlled in order  to prevent solids from passing
 through the filter and into  the effluent.

 Maintainability:   The membrane filters must be  regularly moni-
 tored,  and cleaned or replaced as necessary.  Depending on the
 composition of the waste  stream and  its flow rate,  frequent
 cleaning of the  filters may  be required.  Flushing with hydro-
 chloric acid for  six  to 24 hours  will usually suffice.   In
 addition,  the routine maintenance of pumps,  valves,  and other
 plumbing is  required.

 Solid Waste Aspects:   When the recirculating reagent-precipitate
 slurry  reaches 10  to  15 percent solids,  it  is pumped out of the
 system.   It  can then  be disposed  of  directly to  a landfill  or it
 can undergo  a dewatering  process.  Because  this  sludge  contains
 toxic metals,  it requires proper  disposal.
                                          j
 Demonstration  Status.  There are  more than  25 membrane.filtration
 systems  presently  in  use  on metal finishing and  similar waste-
waters.  Bench scale  and pilot  studies  are  being  run  in an
 attempt  to  expand  the list of  pollutants  for which  this  system is
known to.be  effective.  Although  there  are  no data  on the use  of
 membrane filtration in copper  forming plants, the  concept has
been  successfully  demonstrated using  coil coating plant waste-
water.
                               288

-------
Reverse Osmosis

The process of osmosis involves the passage of a liquid through  a
semipermeable membrane from a dilute to a more concentrated solu-
tion.  Reverse osmosis (RO) is an operation in which pressure  is
applied to the more concentrated solution, forcing the permeate
to diffuse through the membrane and into the more dilute  solu-
tion.  This filtering action produces a concentrate and a perme-
ate on opposite sides of the membrane.  The concentrate can then
be further treated or returned to the original production opera-
tion for continued use, while the permeate water can be recycled
for use as clean water.  Figure VII-30 depicts.a reverse  osmosis
system.

As illustrated in Figure VII-31, there are three basic configura-
tions used in commercially available RO modules:  tubular,
spiral-wound, and hollow fiber.  All of these operate on  the
principle described above, the major difference being their
mechanical and structural design characteristics.

The tubular membrane module uses a porous tube with a cellulose
acetate membrane-lining.  A common tubular module consists of  a
length of 2.5 cm (1 inch) diameter tube wound on a supporting
spool and encased in a plastic shroud.  Feed water is driven into
the tube under pressures varying from 40 to 55 atm (600 to 800
psi).  The permeate passes through the walls of the tube  and is
collected in a manifold while the concentrate is drained  off at
the end of the tube.  A less widely used tubular RO module uses  a
straight tube contained in a housing, under the same operating
conditions.

Spiral-wound membranes consist of a porous backing sandwiched
between two cellulose acetate membrane sheets and bonded  along
three edges.  The fourth edge of the composite sheet is attached
to a large permeate collector tube.  A spacer screen is then
placed on top of the membrane sandwich and the entire stack is
rolled around the centrally located tubular permeate collector.
The rolled up package is inserted into a pipe able to withstand
the high operating pressures employed in this process, up to 55
atm  (800 psi) with the spiral-wound module.  When the system is
operating, the pressurized product water permeates the membrane
and flows through the backing material to the central collector
tube.  The concentrate is drained off at the end of the container
pipe and can be reprocessed or sent to further treatment  facili-
ties.

The hollow fiber membrane configuration is made up of a bundle of
polyamide fibers of approximately 0.0075 cm  (0.003 in.) OD and
0.043 cm  (0.0017 in.) ID.  A commonly used hollow fiber module
contains several hundred thousand of the fibers placed in a long
                               289

-------
 tube, wrapped  around a flow screen,  and rolled into a spiral.
 The  fibers  are bent  in a U-shape and their ends are supported  by
 an epoxy  bond.   The  hollow fiber unit is operated under 27  atm
 (400 psi),  the feed  water  being dispersed from the center of the
 module  through a porous distributor  tube.  Permeate flows through
 the  membrane to  the  hollow interiors of the fibers and is col-
 lected  at the  ends of the  fibers.         .

 The  hollow  fiber and spiral-wound modules have a distinct advan-
 tage over the  tubular system in that they are  able to load  a very
 large membrane surface area into a relatively  small volume.  How-
 ever, these two  membrane types  are much more susceptible to foul-
 ing  than  the tubular system,  which has  a larger flow channel.
 This characteristic  also makes  the tubulajr membrane much easier
 to clean  and regenerate than either  the spiral-wound or hollow
 fiber modules.   One  manufacturer claims that their helical
 tubular module can be physically wiped  clean by passing a soft
 porous  polyurethane  plug under  pressure through the module.

 Application and  Performance.  In a number of metal processing
 plants, the overflow from  the first  rinse in a countercurrent
 setup is  directed to a reverse  osmosis  unit, where it is sepa-
 rated into  two streams.  The concentrated stream contains dragged
 out  chemicals  and is returned to th6 bath to replace the loss  of
 solution  due to  evaporation and dragout.  ! The  dilute stream (the
 permeate) is routed  to the last rinse tank to  provide water for
 the  rinsing operation.   The rinse flows from the last tank  to  the
 first tank  and the cycle is  complete.

 The closed-loop  system described above  may be  supplemented  by  the
 addition  of a  vacuum evaporator after the RO unit in order  to
 further reduce the volume  of  reverse osmosis concentrate.   The
 evaporated  vapor can be condensed and returned to the last  rinse
 tank or sent on  for  further  treatment.    ;

 The largest application has been for the  recovery of nickel  solu-
 tions.  It  has been  shown  that  RO  can generally be applied  to
 most acid metal  baths  with a  high  degree  of performance,  provid-
 ing that  the membrane unit is not  overtaxed.   The limitations
 most critical here are the allowable pH range  and maximum operat-
 ing pressure for each particular configuration.
                                          j
Adequate prefiltration is  also  essential.;  Only three membrane
 types are readily available in  commercial RO units,  and  their
 overwhelming use has been  for the  recovery of  various acid  metal
 baths.  For the  purpose of calculating  pei-formance predictions  of
 this technology,   a rejection  ratio of 98  percent  is  assumed  for
 dissolved salts,  with 95 percent permeate recovery.
                               290

-------
Advantages and Limitations.  The major advantage of reverse osmo-
sis tor handling process effluents Is its ability to concentrate
dilute solutions for recovery of salts and chemicals with  low  ^
power requirements.  No latent heat of vaporization or  fusion  is
required for effecting separations; the main  energy requirement
is for a high pressure p\imp.  It requires relatively little , floor
space for compact, high capacity units, and it  exhibits good
recovery and rejection rates for a number of  typical process
solutions.  A limitation of the reverse osmosis process for
treatment of process effluents is its limited temperature  range
for satisfactory operation.  For cellulose acetate  systems, the
preferred limits are 18°C to 30°C (65°F to 85°F); higher tempera-
tures will  increase the rate of membrane hydrolysis and reduce
system life, while lower temperatures will result^in decreased
fluxes with no  damage  to the membrane.  Another limitation is
inability to handle certain solutions.  Strong  oxidizing agents,
strongly  acidic or basic solutions,  solvents, and other organic
compounds can cause dissolution of  the  membrane.  Poor  rejection
of some  compounds  such as  borates and  low molecular weight organ-
ics is another  problem.  Fouling of membranes by slightly  soluble
components  in  solution or  colloids  has  caused failures, and foul-
ing of membranes by  feed waters with high  levels of suspended
solids  can  be  a problem.   A. final  limitation is inability  to
treat or  achieve high  concentration with  some solutions.  Some
concentrated  solutions may have  initial osmotic pressures  which
are so high that they  either  exceed available operating pressures
or are  uneconomical  to treat.

Operational Factors.   Reliability:   Very good reliability is  _
 achieved so long as  the proper precautions  are taken to minimize ,
 the chances of fouling or degrading the membrane.   Sufficient
 testing of the waste stream prior to application of an RO system
 will provide the information needed to insure  a successful
 application.

 Maintainability:  Membrane life is estimated to range  from six
 months to three years, depending on the use  of the system.  Down
 time for flushing or cleaning is on the order  of two hours as
 often as once  each week; a substantial portion of maintenance
 time must be spent on cleaning any prefilters  installed ahead of
 the reverse osmosis unit.

 Solid Waste Aspects:  In a closed loop system  utilizing RO there
 is a constant  recycle of permeate and a minimal amount of solid
 waste.  Prefiltration eliminates many solids before they  reacn
 the module and helps keep the buildup to a minimum.  These solids
 require proper disposal.
                                291

-------
 Demonstration Status.  There  are presently at  least  one hundred
 reverse osmosis wastewater applications in a variety of indus-
 tries.  In addition to these, there are 30 to  40 units being used
 to provide pure process water for several industries.  Despite
 the many types and configurations of membranes, only the spiral-
 wound cellulose acetate membrane has had widespread success in
 commercial applications.  One copper forming plant currently uses
 reverse osmosis.

 Sludge Bed Drying
 ..... -'— ^ ...........  ..i  ^  , ,.«                         |

 As a waste treatment procedure,  sludge bed drying is employed to
 reduce the water content of a variety of sludges to the point
 where they are amenable to mechanical collection and removal to a
 landfill.   These beds usually consist of 15 to 45 cm (6 to 18
 in.)  of sand over a 30 cm (12 in.)  deep gravel drain system made
 up of 3 to 6 mm (1/8 to 1/4 in.) graded gravel overlying drain
 tiles.  Figure VII-32 shows the  construction of a drying bed.
                                           I
 Drying beds are usually divided  into sectional areas approxi-
 mately 7.5 meters ^ (25 ft)  wide x 30  to 60 meters (100 to 200 ft)
 long.   The partitions may  be  earth  embankments, but more often
 are made of planks  and supporting grooved posts.

 To apply liquid sludge to  the sand bed,  a closed conduit or a
 pressure pipeline with valved outlets  at  each sand  bed  section is
 often employed.   Another method  of application is by means  of  an
 open  channel  with appropriately  placed  side  openings  which  are
 controlled by slide  gates.  With either type  of delivery system
 a  concrete  splash slab should be provided  to  receive  the  falling
 sludge and prevent erosion of the sand  surface.
                                           i
 Where  it is necessary  to dewater sludge  continuously  throughout
 the year regardless of the weather,  sludge beds may be  covered
 with a fiberglass reinforced  plastic or other roof.   Covered
 drying beds permit a greater  volume of  sludge  drying  per year  in
 most climates because  of the  protection afforded from rain  or
 snow and because of more efficient control of  temperature.
 Depending on  the  climate,  a combination of open and  enclosed beds
 will prova.de maximum utilization of the sludge  bed drying facili-
Application and Performance.  Sludge drying beds are a means of
dewatering sludge from clarifiers and thickeners.  They are
widely used both in municipal and industrial treatment facili-
ties.

Dewatering of sludge on sand beds occurs by two mechanisms:  fil
tration of water through the bed and evaporation of water as a
result ^of radiation and convection.  Filtration is generally com
plete in one to two days and may result in solids concentrations
                               292

-------
as high as 15 to 20 percent.  The rate of filtration depends on
the drainability of the sludge.

The rate of air drying of sludge is related to temperature, rela-
tive humidity, and air velocity.  Evaporation will proceed at a
constant rate to a critical moisture content, then at a falling
rate to an equilibrium moisture content.  The average evaporation
rate for a sludge is about 75 percent of that from a free water
surface.

Advantages and Limitations.  The main advantage of sludge drying
beds over other types of sludge dewatering is the relatively low
cost of construction, operation, and maintenance.

Its disadvantages are the  large area of land required and long
drying times that depend, to a great extent on climate and
weather.

Operational Factors.  Reliability:  Reliability is high with
favorable climatic conditions, proper bed design, and^care to
avoid excessive or unequal  sludge  application.  If climatic con-
ditions in a given area are not favorable for adequate drying,  a
cover may be necessary.

Maintainability:  Maintenance  consists  basically  of  periodic
removal of the dried  sludge.   Sand removed  from the  drying bed
with  the  sludge must  be replaced  and the  sand  layer  resurfaced.

The resurfacing of  sludge  beds is  the major expense  item  in
sludge bed maintenance, but there  are other areas which may
require attention.  Underdrains  occasionally become  clogged  and
have  to be cleaned.   Valves or sludge gates that  control  the  flow
of sludge to  the  beds must be  kept watertight.  Provision for
drainage  of  lines in  winter should be provided  to prevent damage
from  freezing.  The partitions between  beds should  be tight.so
that  sludge  will  not  flow  from one compartment  to another.^  The
outer walls  or banks  around the beds  should also  be  watertight.

Solid Waste  Aspects:   The  full sludge  drying bed  must either^be
abandoned or the  collected solids must  be removed to a landfill.
These solids contain  whatever metals  or other materials  were
 settled in the clarifier.   Metals will  be present as hydroxides,
 oxides,  sulfides, or  other salts.   They have the  potential for
 leaching  and contaminating ground water,  whatever the location of
 the semidried solids.  Thus the abandoned bed or landfill should
 include provision for runoff control and leachate monitoring.

 Demonstration Status.  Sludge beds have been in common use in
 both municipal and industrial facilities for many years.   How-
 ever, protection of ground water from contamination is not always
 adequate.
                                293

-------
 Ultrafiltration
                                          i
 Ultrafiltration (UF) is a process which uses semipermeable poly-
 meric membranes to separate emulsified or colloidal materials
 suspended in a liquid phase by pressurizing the liquid so that it
 permeates the membrane.  The membrane of an ultrafilter forms a
 m?ifcular screen which retains molecular particles based on their
 differences in size, shape, and chemical structure.  The membrane
 permits passage of solvents and lower molecular weight molecules.
 At present, an ultrafilter is capable of removing materials with
 molecular weights in the range of 1,000 to 100,000 and particles
 of comparable or larger sizes.

 In an Ultrafiltration process, the feed solution is pumped
 through a tubular membrane unit.   Water and some low molecular
 weight materials pass through the membrane under the applied
 pressure of 10 to 100 psig.  Emulsified oil droplets and sus-
 pended particles are retained, concentrated,  and removed continu-
 ously.   In contrast to ordinary filtration,  retained materials
 are washed off the membrane filter rather than  held by it.
 Figures VII-33 and VII-34 represent the Ultrafiltration process.
                                          ]
 Application and Performance.   Ultrafiltration has  potential
 application to aluminum forming plants  for  separation of oils and
 residual solids from a variety of waste streams.   In treating
 aluminum forming wastewater its greatest applicability would be
 as  a polishing treatment  to remove residual precipitated metals
 after chemical precipitation  and  clarification.  Successful
 commercial use,  however,  has  been primarily  for separation  of
 emulsified oils  from wastewater.   Over  one hundred such units
 operate in the United States,  treating  emulsified  oils  from
  now
a
variety of industrial processes.  Capacities  of  currently oper-
ating units range  from a  few hundred  gallons  a week  to 50,000
gallons per day.   Concentration of oily emulsions to 60 percent
oil or more are possible.  Oil concentrates of 40 percent or more
are generally suitable for incineration, and  the permeate can be
treated further and in some cases recycled back  to the process.
In this way, it is possible to eliminate contractor removal costs
tor oil from some  oily waste streams.

Table VII-28 indicates Ultrafiltration performance (note that UF
is not intended to remove dissolved solids).  The removal
percentages shown  are typical, but they can be influenced by pH
and other conditions.  The high TSS level is unusual for this
technology and Ultrafiltration is assumed to reduce the TSS level
by one-third after mixed media filtration.[
                               294

-------
The permeate or effluent from the ultrafiltration unit is nor-
mally of a quality that can be reused in industrial applications
or discharged directly.  The concentrate from the ultrafiltration
unit can be disposed of as any oily or solid waste.

Advantages and Limitations.  Ultrafiltration is sometimes an
attractive alternative to chemical treatment because  of lower
capital equipment, installation, and operating costs, very high
oil and suspended solids removal, and little required pretreat-
ment.  It places a positive barrier between pollutants and
effluent which reduces the possibility of  extensive pollutant  ^
discharge due to operator error or upset in settling  and  skimming
systems.  Alkaline values in alkaline cleaning solutions  can be
recovered and reused in the process.

A  limitation of ultrafiltration for treatmentQof  process
effluents is its narrow temperature range  (18 C to  30 C;  for
satisfactory operation.  Membrane life decreases  with higher
temperatures, but  flux increases  at elevated  temperatures.
Therefore, sxirface area requirements are a function of tempera-
ture  and become  a  tradeoff between  initial costs  and  replacement
costs  for the membrane.  In  addition, ultrafiltration cannot
handle certain  solutions.  Strong oxidizing agents,  solvents,  and
other  organic compounds can  dissolve  the membrane.  Fouling is
sometimes  a  problem,  although  the high  velocity  of the wastewater
normally creates enough turbulence  to keep fouling at a  minimum.
Large solids particles can sometimes  puncture the membrane and
must  be removed by gravity  settling or  filtration prior  to the
ultrafiltration unit.

Operational  Factors.   Reliability:   The reliaiblity of an ultra-
 filtration system is  dependent on the proper filtration,  set-
 tling  or other treatment of incoming waste streams to prevent_
 damage to  the membrane.   Careful pilot studies should be done in
 each instance to determine necessary pretreatment steps and the
 exact membrane type to be used.   It: is advisable to remove any
 free, floating oil prior to ultrafiltration.  Although free oil
 can be processed,  membrane performance may deteriorate.

 Maintainability:  A limited amount of regular maintenance is
 required for the pumping system.  In addition, membranes must be
 periodically changed.  Maintenance associated with membrane^
 plugging can be reduced by selection of a membrane with  optimum
 physical characteristics and sufficient velocity of  the waste
 stream.  It is often necesary to occasionally pass a detergent
 solution through the system to remove an  oil and grease  film
 which  accumulates on  the membrane.  With  proper  maintenance,
 membrane life can be greater than 12 months.
                                295

-------
 Solid Waste Aspects:   Ultrafiltration is used primarily to
 recover  solids  and liquids.   It therefore eliminates solid waste
 problems when the solids (e.g., paint solids) can be recycled to
 the  process.   Otherwise, the stream containing solids must be
 treated  by end-of-pipe equipment.   In the most probable applica-
 tions within the aluminum forming  category,  the ultrafilter would
 remove concentrated oily wastes which can be recovered for reuse
 or used  as a fuel.

 Demonstration Status.   The ultrafiltration-process is well devel-
 oped and commercially  available for treatment of wasteiwater or
 recovery of certain high molecular weight liquid and solid con-
 taminants.  Currently,  no plants in the copper forming category
 use  ultrafiltration.   One aluminum forming plant ultrafilters its
 spent rolling oils.  Ultrafiltration is well suited for highly
 concentrated  emulsions,  for  example, rolling and drawing oils,
 although it is  not suitable  for free oil.

 Vacuum Filtration
                                           i
 In wastewater treatment  plants, sludge dewatering by vacuum fil-
 tration  generally uses  cylindrical drum filters.  These drums
 have a filter medium which may be  cloth made of natural or syn-
 thetic fibers or a wire-mesh fabric.  The drum is suspended above
 and  dips into a vat of  sludge.   As the drum rotates slowly, part
 of its circumference is  subject to an internal vacuum that draws
 sludge to  the filter medium.   Water is drawn through the porous
 filter cake thorugh the  drum fabric to a discharge port, and the
 dewatered  sludge,  loosened by compressed air, is scraped from the
 filter mesh.  Because the dewatering of sludge on vacuum filters
 is relatively expensive  per  kilogram of water removed,  the liquid
 sludge is  frequently thickened  prior to processing.  A vacuum
 filter is  shown in Figure VII-35.

Application and Performance.   Vacuum filters are frequently used
both in  municipal  treatment  plants and in a  wide variety of
 industries.   They are most commonly used in  larger facilities,
which may  have  a thickener to double the sqlids  content of clari-
 fier sludge before  vacuum filtering.  Often  a precoat is used to
 inhibit  filter  blinding.

The  function  of vacuum filtration  is to reduce the water content
of sludge,  so that  the solids content increases  from about 5
percent  to  between  20 and 30 percent,  depending  on the  waste
characteristics.

Advantages  and  Limitations.   Although the initial cost  and area
requirement of  the vacuum filtration system  are  higher  than those
of a centrifuge,  the operating  cost is lower,  and no special pro-
visions  for sound  and vibration protection ineed  be made.   The
                               296

-------
de-watered sludge from this process is in the form of a moist cake
and can be conveniently handled.
Operational Factors.  Reliability:  Vacuum filter systems      ^
proven reliable at many industrial and municipal treatment facil-
ities.  At present, the largest municipal installation is^at^the
West Southwest wastewater treatment plant of Chicago, Illinois,
where 96 large filters were installed in 1925, functioned approx-
imately 25 years, and then were replaced with larger units.
Original vacuum filters at Minneapolis-St. Paul, Minnesota now
have over 28 years of continuous  service, and Chicago has some
units with similar or greater service life.

Maintainability:  Maintenance consists of the cleaning or
replacement of the filter media,  drainage grids, drainage piping,
filter pans, and other parts of the equipment.  Experience in  a
number of vacuum filter plants indicates that maintenance
consumes approximately 5 to 15 percent of the total time.  If
carbonate buildup or other problems are unusually  severe, mainte-
nance time may be as high as 20 percent.  For this reason, it  is
desirable to maintain one or more spare units.

If  intermittent operation is used,  the filter equipment  should be
drained and washed each time it is  taken out of service.  An
allowance for this wash time must be  made  in  filtering  schedules.

Solid Waste Aspects:  Vacuum filters  generate a solid cake which
is  usually trucked  directly to landfill.  All of the metals
extracted from  the  plant wastewater are  concentrated in the
filter cake as hydroxides, oxides,  sulfides, or other salts.

Demonstration Status.  Vacuum  filtration has been  widely used  for
many years.  It  is  a  fully proven,  conventional technology  for
sludge dewatering.  Several copper forming  plants  report its use.

IN-PLANT  CONTROL TECHNIQUES  (FLOW REDUCTION)

This section presents  a discussion of flow  reduction techniques
which are applicable  to  copper forming plants  for  the purpose  of
reducing  the volume of wastewater discharged  to treatment.   Flow
reduction is  a  control technique  which,  in conjunction  with the
treatment processes previously discussed,  can further reduce the
mass of  pollutants discharged.  The primary flow  reduction
techniques  which are  applicable  to copper forming  plants are
recycle,  alternative  rinsing  techniques,  particularly  spray
rinsing  and counter cur rent  rinsing, contract  hauling and
 reduction of water use.
                                297

-------
 Recycle                                    j

 Nearly all copper forming plants recycle some process wastewater
 streams.  The most commonly reeyelecL streams include spent lubri-
 cating solutions, annealing contact cooling water and solution
 heat treatment contact cooling water.  In general, some treatment
 is required to allow process wastewater recycle in this industry
 but the required treatment is generally less than that needed for
 discharge.  At present, the  most common treatment practices
 prior to recycle in copper forming plants are suspended solids
 removal, oil skimming, and cooling.  Wastewater is most often
 returned to the process operation from which it originated, but
 may also be used in other operations.

 Recycle is highly effective in reducing pollutant discharges,
 often eliminating the discharge completely.  Where a discharge
 remains, the volume requiring treatment is greatly reduced,
 making the application of advanced treatment techniques more
 economically attractive.   Recycle often results in considerably
 reduced requirements  for process materials  and corresponding
 reductions in raw waste loads for some pollutants (e.g.,  oil and
 grease and toxic organics  in soluble oil systems).

 Where recycle is presently practiced,  the rate of recycle  varies
 from approximately 30 to 100 percent.   Many copper forming plants
 currently achieve zero discharge of some waste streams  through
 natural evaporation or land application;  however,  these options
 are not available to  all plants  in the industry.   The Agency
 recognizes that  discharge  of wastewater from particular sources
 may not be avoided.   This  is  discussed in greater  detail in the
 context of specific sources.
                                            i
 Cold  Rolling, Hot Rolling  and Drawing  Lubricants.  Lubricants
 used  in cold rolling  and drawing are commonly recycled  to  such an
 extent  that contract  removal  of  the  total discharge  is  practical.
 Factors which limit the extent of recycling  include heat removal,
 degradation of lubricants  which  results in  staining  of  the
 product,  or build-up  of dissolved or suspended  solids.  These
 limitations may  often be overcome by the  application  of more
 advanced  treatment techniques than those presently in common  use
 for recycle as discussed below.

The use of water  soluble oil and emulsified  oil lubricants  in
 cold  rolling processes makes it  easier  to recycle lubricants  than
 in  cases where non-emulsified oil--water mixtures are in use.  In
addition,  most drawing operations use emulsified lubricants.
Emulsified  lubricants  are  commonly used repeatedly and dumped
when  contamination forces replacement of the  solution.  This type
of  technology uses much less process water and oil on a yearly
                               298

-------
basis than most processes which have continuous oil—water mix-
ture applications; therefore, both process material costs and
treatment or disposal costs can be reduced.

The most common problems encountered in the use of soluble oil
lubricants are the accumulations of heavy metals  (especially
copper) and other suspended solids, and the degradation of the
emulsion due to heat and stress.  Several methods are used to
prolong the life of the solutions, resulting in even lower   ^
end-of-pipe treatment and/or disposal costs.  Most recalculating
lubricant systems have a storage tank from which  the lubricant  is
drawn and to which it is returned following application to the
process material.  This storage tank serves the dual purpose of
allowing solids to settle and the lubricant to cool prior to
recycle.  Some of these tanks are baffled to enhance settling.
In some copper and copper alloy plants, paddle type devices
traveling on a conveyorized belt, scrape out, solids which
accumulate on the bottom of lubricant recirculation tanks. This
helps to minimize the contamination of  the  lubricant by avoiding
the build-up of solids on the bottom of the tank.  The sludge
removed is often  rich enough  in copper  fines to be sent out  for
reclamation.  Cartridge and membrane filtration is also known  to
remove solids from lubricant  streams. These filters^must be
cleaned or replaced as they become clogged  with solids.

Annealing Contact Cooling Water.  Annealing quenches using only
water are commonly recycled."Treatment  of annealing  quench
water prior to recycle is typically limited to settling and  heat
removal; however, many sites  reported  recycle with no  prior
treatment.

Because annealing quench  operations are characteristically
intermittent, retention  and  equalization tanks  are generally^
required  for recycle.  These  tanks  can also serve as  a settling
basin  for  removal of  suspended  solids  and sufficient  cooling and
temperature  equalization  to  allow a significant  degree of  recycle
without  addition of  non-contact cooling or the  use of a cooling
tower.

Total  recycle may be  prohibited by the presence  of dissolved
 solids  for plants which  can not take  advantage  of natural  evap-
 oration  or  land  application.   Dissolved solids  (e.g.,  sulfates
 and chlorides)  entering  a totally recycled waste stream may
 precipitate,  forming scale  if the solubility  limits  of the
 dissolved solids are exceeded.   A bleed stream may be necessary
 to prevent maintenance problems (pipe plugging or scaling, etc.;
 that would be created by the precipitation of dissolved solids.

Required hardware necessary for recycle is highly site-specific.
 Recycling through cooling towers is the most common practice.
                                299

-------
 Basic Items include the cooling tower, pumps and piping.  Addi-
 tional materials are necessary if water treatment occurs before
 the water is recycled.  Chemicals may be necessary to control
 scale buildup,  slime, and corrosion problems, especially with
 recycled cooling water.  Maintenance and energy use are limited
 to that required by the pumps, and solid waste generation is
 dependent on the type of treatment system in place.  A typical
 flow diagram for a system using a cooling tower to recycle water
 is shown in Figure VII-36.

 Solution Heat Treatment Contact Cooling Water.  Water quenches
 (solution heat  treatment) are widely used in copper forming
 plants following hot deformation processes to rapidly reduce
 product temperatures in order to limit surface oxidation and
 allow safe handling of the material.  The quench water becomes
 contaminated with metals, suspended solids,  and lubricants, but
 the primary effect of this use is elevation of the water tempera-
 ture.   Because  only minor chemical changes! are produced in the
 quench solutions, extensive recycle and reuse is possible without
 deleterious effects on production.

 In general,  quench water associated with solution heat treatment
 produces relatively large volumes of water which contain low
 concentrations  of pollutants.   As a result treatment effective-
 ness  is somewhat limited unless in-process control techniques are
 employed.   Recycle and reuse of the quench water and a reduction
 of water use can reduce the volume of effluent requiring treat-
 ment  and increase pollutant concentrations to more treatable
 levels.

 Alternative Rinsing Techniques
Reductic i  in  the  amount  of water  used  and (discharged in copper
and copper alloy  manufacturing  can be  realized  through the
installation  and  use  of  efficient rinsing techniques.   The tech-
niques discussed  are  alternatives to stagnant rinsing.   These
techniques can result in water  cost savings, reduced waste treat-
ment chemical costs and  improved  waste treatment  efficiency.   The
design of  rinse systems  for minimum water use depends  on the
maximum level of  contamination  allowed to remain  on  the work
piece (without reducing  product quality)  as well  as  on the
efficiency or effectiveness of  each rinse stream.
                                           i

Rinsing is used to dilute  the concentration of  contaminants
adhering to the surface  of a workpiece to an acceptable level
before the workpiece  passes on  to the  next,step of a pickling
operation.  The amount of  water required  to dilute the  rinse
solution depends  on the  quantity  of chemical drag-in from the
upstream rinse or pickling tank,  the allowable  concentration  of
chemicals  in the  rinse water, and the  contacting  efficiency
between the workpiece and  the water.
                               300

-------
Counter-current Cascade Rinsing

Process variations such as countercurrent cascade rinsing may
cause a decrease in process water use.  This technique reduces
water use by countercurrent multiple stage rinsing of the copper
products.  Clean rinse water first contacts the copper in the
last stage.  The water, somewhat more contaminated, is routed
stage by stage up the rinsing line.  After use in the first rinse
stage, the contaminated water is discharged to treatment.

As an example, Figure VII-37 illustrates three rinsing opera-
tions, each designed to remove the residual acid in the water on
the surface of a workpiece.  In Figure VII-37a the piece is
dipped into one tank with continuously flowing water.  In this
case, the acid on the surface of the workpiece is essentially
diluted to the required level.

In Figure VII-37b, the first step towards countercurrent opera-
tion is taken with the addition of a second tank.  The workpiece
is now moving in a direction opposite to the rinse water.  The
piece is rinsed with fresh makeup water prior to moving down the
assembly line.  However, the fresh water from this final rinse
tank is directed to a second tank, where it meets the incoming,
more-contaminated workpiece.  Fresh makeup water is used to give
a final rinse to the article before it moves out of the rinsing
section, but the slightly contaminated water is reused to clean
the article just coming into the rinsing section.  By increasing
the number of stages, as shown in Figure VII-37c, further water
reduction  can be achieved.  Theoretically,  the amount of water
required is the amount of acid being removed by single-stage
requirements divided by the highest tolerable concentration  in
the outgoing rinsewater.  This theoretical  reduction of water by
a countercurrent multistage operation  is shown in the curve  graph
in Figure VII-38.  The actual  flow reduction obtained is a
function of the dragout and the type  of  contact occurring  in the
tanks.  If reasonably good contact is  maintained major reductions
in water use are possible.

Significant flow reductions can be achieved by the  addition  of
only one additional stage in the rinsing operation, as discussed
above.  As  shown  in Figure VII-38  the  largest  reductions  are made
by adding  the first few stages.  Additional rinsing stages cost
additional money.  The  actual  number  of  stages added  depends  on
site-specific layout and  operating conditions.  With higher  costs
for water  and waste treatment, more  stages  might be economical.
With very  low water costs,  fewer  stages  would be economical.   In
considering retrofit  applications,  the space  available  for
additional tanks  is also  important.   Many  other  factors  will
affect  the economics  of countercurrent cascade  rinsing;  an
evaluation must be done for each  individual plant.
                               301

-------
 Rinse water requirements and the benefits of countercurrent rins-
 ing  may  be  influenced by the volume of solution dragout carried
 into each rinse stage by the material being rinsed, by the number
 of rinse stages used, by the initial concentrations of impurities
 being removed,  and by the final product cleanliness required.
 The  influence of these factors is expressed in the rinsing
 equation which  may be stated simply as:
     Vr
                   x VD
     Vr  is  the  flow through each rinse stage.
     Co  is  the  concentration of the contaminant(s)  in the initial
         process bath.
     Cf  is  the  concentration of the contaminant(s)  in the final
         rinse to  give  acceptable product  cleanliness.
      n  is  the  number  of rinse  stages  employed.
     VD  is  the  dragout carried  into each  rinse stage, expressed
         as  a flow.

For a multi-stage rinse,  the total  volume of rinse  wastewater is
equal to n  times  Vr while for a countercurrent rinse the total
volume of wastewater discharge  equals  Vr.   Drag-out is solution
which remains on  the .surface of material  being rinsed when it is
removed  from process baths  or rinses.       i
                                            i
In the copper forming  category,  countercurrent cascade rinsing
can be applied to pickling  and  alkaline cleaning  rinsing
operations.  To calculate the benefits of countercurrent rinsing
for copper  forming,  it can  be assumed  that a two-stage
countercurrent cascade rinse is  installed after pickling.   The
mass of copper in one  square meter  of  sheet that  is 6 mm
(0.006 m) in thickness can  be calculated  using the  density of
copper, 8.90 kkg/m3 (556  Ibs/cu  ft), as follows:

- (0.006 m) x   (8.90 kkg/m3)  =  0.053 kkg/m2 of sheet

Using the mean pickling rinse water use from Table  V-12 (p. 97  ),

Vr can then be calculated as  follows:
Vr -  [0.053  kkg   x   4,000
      \         m^
      \

   -  213.6  1/m2 of sheet.
                              1 \
                             EEgj
                               302

-------
If the film on a piece of copper sheet is 0.015 mm  (0.6 mil)
thick, (equivalent to the film on a well-drained vertical
surface) then the volume of process solution, VD, carried  into
the rinse tank on one square meter of sheet will be:

VD =  (0.015 mm)  x /	1  m/mm\ x  (1000 1/m3)
                   \TOUO~     /

= 0.015 1/m2 of sheet

Let r = Go, then r 1/n = Vr
        CT               VD

For single stage rinsing n = 1

Therefore r == Vr
              W

and r = 213.7 = 14,240
        U7TJT5

For a 2-stage countercurrent cascade  rinse  to  obtain the  same r,
that  is the same product cleanliness,

      Vr = r^/2 and:
     W
             119.3


But VD  =  0.015  1/m2  of sheet
Vr
VD
Therefore  for  2-stage countercurrent cascade rinsing Vr is:

     Vr    =  119.3  x  0.015  =  1.79 1/m2 of sheet.

In  this  example,  two-stage countercurrent rinsing achieved 99.2
percent  reduction in the water used.  The actual numbers may vary
depending  on efficiency of squeegees or air knives, and the rinse
ratio  desired.

Countercurrent cascade rinsing has been widely used as a flow
reduction  technique in the metal finishing industry.  Counter-
current  cascade rinsing is currently practiced at^four copper
forming  plants.  In aluminum conversion coating lines that are
subject  to the coil coating limitations, countercurrent cascade
rinsing  is currently used in order to reduce costs of wastewater
treatment  systems (through smaller systems) for direct dis-
chargers and to reduce sewer costs for indirect dischargers.
                                303

-------
 Spray Rinsing        ,                      ;

 Spray rinsing is  another method used to dilute the concentration
 of  contaminants adhering to the surface of a workpiece.   The
 basis of this approach  is to spray water onto the surface of the
 workplace, as  opposed  to submerging it into a tank.  The  amount of
 water contacting  the  workpiece is  minimized as is the amount of
 water discharged.   The  water use and discharge rates can be
 further  reduced through recirculation of the rinse water.  Copper
 forming  plants practicing spray rinsing discharge typically 60
 percent  less  water than those plants using only stagnant rinses.

 The equipment required  for spray rinsing includes piping, spray
 nozzles,  a pump,  a holding tank,  and a collection basin.  The
 holding  tank  may  serve  as the collection basin to collect the
 rinse water prior to  recirculation as a method of space  economi-
 zation.
                                            i
 Contract Hauling

 Contract hauling  refers to the industry practice of contracting a
 firm to  collect and transport wastes for off-site disposal.   This
 practice is particularly applicable to low-Volume, high  concen-
 tration  waste streams.   Examples of such waste streams in the
 copper forming industry are pickling baths,  drawing lubricants,
 cold rolling  lubricants,  annealing oil and extrusion press solu-
 tion heat treatment.                        :

Reduction of  Water Use

The  reduction of  process  water use has been  found to be  an
effective approach to reducing treatment costs and pollutant dis-
charges  at many copper  forming plants.   In most cases, substan-
tial reduction may be achieved by  simple actions  involving little
or no cost.   It is  often  found that satisfactory operation may be
achieved  with much smaller rinse or contact  cooling water flows
than have generally been  used.  Many of the  copper forming plants
visited reported recent  significant reductions in process water
use  and  discharge.

Many production units in  copper forming plants operate intermit-
tently or at  widely varying production rateS.   The practice  of
shutting  off  process water streams  during periods when the unit
is inoperative and  of adjusting flow rates during periods of low
activity  can  prevent much unnecessary dilution of wastes and
reduce the volume  of water to  be treated and  discharged.   Water
may be shut off and adjusted  manually or through  automatically
controlled valves.  Manual  adjustment  involves  minimal capital
cost and  can  be just as reliable in actual practice.  Automatic
                               304

-------
shut off valves are used in some copper forming^operations to
turn off water flows when production units are inactive.  Auto-
matic adjustment of flow rates according to production
-------
 are also used to reduce drag-out from soap and other lubricant
 tanks which are often found as a final step in automatic strip
 lines.                                                       v
                                            i
                                            i
 Heating the tank containing the process bath can also help reduce
 drag-out of process solutions in two ways:  by decreasing the
 viscosity and the surface tension of the solution.   A lower
 viscosity allows the liquid to flow more rapidly and therefore
 drain at a faster rate from the product following application in
 a process bath.   Increasing 'the temperature of the  solution
 decreases its viscosity,  thereby reducing the amount of process
 solution which is dragged out into succeeding rinses.   Likewise,
 a higher temperature will result in lower surface tension in the
 solution.  The amount of  work required to overcome  the adhesive
 force between a liquid film and a solid surface is  a function of
 the surface tension of the liquid and the contact angle.   Lower-
 ing the surface tension reduces the amount of work  required to
 remove the liquid and reduces the edge effect (the  bead of liquid
 adhering to the edges of  a product).

 Operator performance can  have a substantial: effect  on  the amount
 of drag-out which results  from manual dip t|ank processes.   Spe-
 cifically,  proper draining time and techniques can  reduce the
 amount of process solution dragged out into rinses.  After dip-
 ping the material into the process tank,  drag-out can  be  reduced
 significantly by simply suspending the product above the  process
 tank while solution drains off.   Fifteen to 20 seconds  generally
 seems  sufficient to accomplish this.   When processing  tubing,
 especially,  lowering one  end of the load during this drain time
 allows  a larger  amount of  solution to run off from  inside  the
 tubes.

All of  the techniques  which  reduce water use  discussed  in  this
 section may  be used at copper forming plants  to achieve the
 average production normalized flows  at plants which  presently
 discharge excessive amounts  of wastewater to  treatment.

Current Industry Practice

Out  of  18 plants  which reported a  discharge of  annealing water,
 six  currently  practice cooling and  recycle.   Reported recycle
rates range  from 50  to 98  percent.  Of 24  plants which reported
the  use of water for solution heat  treatment,  eight  plants  also
reported  the use  of recycle with recycle  rates  from  85 to  100
percent.

A large  number of plants which practice drawing, cold r-olling or
annealing with oil  reported the practice  of extensive recycling
of the  lubricant  streams with  contract hauling  of the small
                              306

-------
amounts of spent lubricant which is periodically discharged.
Eighteen out of 28 plants which have cold rolling operations
recycle and contract haul, thereby achieving zero discharge.
Similarily, 68 out of 80 plants which have drawing operations
achieve zero discharge through recycle and contract hauling.  For
plants which practice annealing with oil, 23 out of 30 plants
achieve zero discharge of annealing oil through contract hauling.

The use of alternate rinsing techniques in pickling operations
was reported by approximately one-third of the 42 plants which
have pickling operations.  The most frequently reported alternate
rinsing technique for pickling is spray rinsing.  Spray rinsing
of pickling rinse water is practiced in 16 copper forming plants.
Countercurrent rinsing and multi-stage rinsing were also
reported.  Countercurrent rinsing is currently practiced by four
plants in the copper forming industry.
                              307

-------
w
Q
H
X!
O
H
Q

Cd
CO

a

-------
1O
10
                        pH

                   Figure VII-2

   COMPARATIVE SOLUBILITIES OF METAL HYDROXIDES
         AND SULFIDE AS A FUNCTION OF pH
                      309

-------

J















O
























.
O
















o





•
























o

0 0
o
o
0 C
coo


	 O 	

<


-------
  0.40
  0.30
Jt
o"
s
a 0.20
u
-i
  0.10
        \
                                  CAUSTIC SODA
                                                SODA ASH AND

                                                CAUSTIC SODA
                                                                10.3
                           Figure VII-4

               LEAD SOLUBILITY  IN THREE ALKALIES
                              311

-------
INFLUENT
L_J_
(a)
30-40 in-* vlv'SANb-'-":
..'•.V/COARS'

EFFLUENT
(b)
6- 10 ft —
DEPTH
E

/-OVERFLOW
/ TROUGH

1 n n n n rTr
.FINE. :-.-.. ;..•;.;
•'.' .' '!•'•' '.' '•••*
."i •' '*•'•!.'•• ': •
•';';•;"; SANO •'.'•;:
/I .v COARSE'
f
t i EFFLUENT V fNFLU
UHOEHORAIN UNDERORAIN \
CHAMBER — * CHAMBER—*
INFLUENT
, , l~JL^J
(d)
COARSE MEDIA— —$
INTERMIX ZONE— p-
FINER MEDIA— —;:.'•;
FINEST MEDIA 	 -s£

UNDERORAIN
CHAMBER — 1
(THRAc[fE; ~T

-%----.TT 30 -40 in
•VSA'N'OtVv-v:. 1
..*.••.•.*:•:•.'/-. I.

T EFFLUENT

X-SRIT TO
RETAIN / « N
SAND \ /
STRAINER -v
EFFLUENT
4-6ft >
i
ENT UNDEROR/
CHAM8E
1
1
(e)
COARSE MEDIA-—
INTERMIX ZONE-y--
FINER MEDIA— -*-
FINEST MEDIA —
t
i
UNDERDRAW
CHAMBER -

/.•..•nur.'.V'
""**•*' 4* '."• **"•.**' ; "
•'.''.COA'RSE.'-'-
• " - ' w . '
^~
MN \
B — i
INFLUENT
.ANTHRACITE
~;..;.:siLiCA-.-'r
^rrj^.rr.TTh.r^.-j:
1^

!
i
T
28- 48 in
!

\ 1 ^-GARNET S/
\ 'EFFLUENT
                                                            INFLUENT
                           Figure VII-5
                                          \

                      FILTER CONFIGURATIONS
(a) Single-Media Conventional Filter.
(b) Single-Media Upflow Filter.
(c) Single-Media Biflow Filter.
(d)  Dual-Media Filter.
(e)  Mixed-Media (Triple-
    Media)  Filter.
                              312

-------
                                                        JNFUUENT
EFFLUEN
                          STORED
                         BACKWASH
                          WATER
          0  COLLECTION CHAMBER
                                             DRAIN
                              Figure VII-6

                       GRANULAR BED FILTRATION
                                 313

-------
SEDIMENTATION BASIN



         INLET ZONE
                             BAFFLES TO MAINTAIN

                             QUIESCENT CONDITIONS
                                        OUTLET ZONE
   INLET LIQUID
 \.
 SETTLING

.  TRAJECTORY  .

    «._«  • •
                                                         A
                                                        .?

                                                       '
                                           OUTLET LIQUID
                                               BELT-TYPE SOLIDS COLLECTION

                                               MECHANISM
                        SETTLED PARTICLES COLLECTED

                        AND PERIODICALLY REMOVED
CIRCULAR CLARIFIER
                             INLET LIQUID
                                           .CIRCULAR BAFFLE
 SETTLING ZONE.
J'-Tr^,-
  INLET ZONE -
 •  •   V*  • •
-.. . ' V v. %
-•       -
                                             =r-7i T
                                              • ^L_
                                                   ANNULAR OVERFLOW WEIR
*. * 1 V-  • . ' .
  • /. LIQUID
*• WFLOW .'
                                                       OUTLET LIQUID
                                                      •SETTLING PARTICLES
           REVOLVING COLLECTION

           MECHANISM
                          SETTLED PARTICLES

                          COLLECTED AND PERIODICALLY

                          REMOVED
                           SLUDGE DRAWOFF
                             Figure VII-7


              REPRESENTATIVE TYPES OF SEDIMENTATION
                                 314

-------
                                         ZQ;
                                         UJ UJ
UJ
z
<£
CC
«s
0.
UJ
CO
                                                                                        00
                                                                                         I
                                                                                        •H
                                                315

-------
                    oo
                             w
                             o

                             <#
                    CM
                                        CO
                                          CO
                                        Hjz;
                                        £? o
                                        •^ H
                                        oja
                                        H H
                                        X O
                                        oia
                                        
-------
c: o
o*
w  UJ
    0.
O  UJ
H-  03
   CC
   O
              I
                                             I
                                             H
                                             H
                                             i-i
                                             a
o
UJ
u_
i-
UJO

  317
                                                  w

                                                  o
                                                  M
                                                  s

                                                  1

                                                  B
                                                  H
                                                  W
                                                              Hi
                                                              cn
                                                              ,-4
                                                  g
                                                  Si
                                                   H-J
                                                   ptl

-------
      I  I
1 1
                       1  1
    -T-  ! . .1.

                       W
                                       ©
                                                                            CM
                                                                            II
ob
be
Concentration
Raw Wa
Cad
EFFECTIVENESS
ENTAT
                                                                                5M
                                                                                B*l
                                                                                sssl
                                                                                = 1
YDROXIDE PREC
tration
in
e
ns.
               (l/Gui) uoijEHU33uo3 mating paieajj. uiniwpeo
                                       318
Data points with a taw waste con
less than 0.1 mg/i were not includ
treatment effectiveness calculatio

-------
t i
L 1
(
1

































I




































|











































I


























I




i



































































1
























i












































i i
!



























i






t
1



































:

1
i




i





























1












(





























^





)



















t

f


















W














i


I

































i
!
1










©

7>









<"









!
i
i























)











!
|



























































































!>

^v
















































i











































i












!)






)MM
O
uu
«^» i^
|> LU
-5. 2
s O
£ =
2/-vi <£
Ol ^
S ^ ^
g i S s
g = S =3
o « > a I
•• s uu ^y o
S si w si
5 ' =92 =
> ea o cj
1 ^^
« 1
=. S:
'5 u
1 £
" -5
a
X
a
a
o a
v~ >•
—







(j/liui) UOUE41U30U03
                           319

-------

I





































































































1


















©




















1










I








^


	 0 	



©










r—
















































































•









*



3



































©





































































































































2 o «-:
1- O
(|/6iu) uoiiBJiusauoQ iuaniyg ps^eajj^ jaddoj
f ' •' "'•"•"




















(

0"
<3

a srs
ii
M . .
g
53
"o
e>
5
§ s s
" a
UJ
>
to
Concentration (my/!)
VH-13
IDSMEWTATIOK EFFECT
'PER
3 cc « o
IS a ss «
a> ca o
1 1.0
Copper Raw 1
Fl
HYDROXIDE PRECIPITATI
'•• 	 "-^ o
»»
e
o
320

-------
      1
•

                 J	L
                                0
                                                                        o      ^»»


                                                                                u
                                                                                w«

                                                                                £
                                                                                «*•

                                                                                |
                                                                                3
                                                                         '""
                                                                              a
                                                                              U5
   UJ

   at
   >
                                                                                          ui
                                                                                          u.
                                                                                          u.
                                                                                          2
UJ UU
c- w
=3 a
09 O
                                                                                          O.
                                                                                          01
                                                                                          s
                                                                                          X
                                                                                          o

                                                                                          a
                                                                                          >•
    .-s
                              321

-------
                                                   <•*) —
                                                   —. IS)

                                                   If   II
                                                   c/t  «